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 Skyrmion Formation at Lattice Defects and Grain Boundaries Studied by Quantitative Off-Axis Electron Holography.

We use in situ Lorentz microscopy and off-axis electron holography to investigate the formation and characteristics of skyrmion lattice defects and their relationship to the underlying crystallographic structure of a B20 FeGe thin film. We obtain experimental measurements of spin configurations at grain boundaries, which reveal inversions of crystallographic and magnetic chirality across adjacent grains, resulting in the formation of interface spin stripes at the grain boundaries. In the absence of material defects, we observe that skyrmions lattices possess dislocations and domain boundaries, in analogy to atomic crystals. Moreover, the distorted skyrmions can flexibly change their size and shape to accommodate local geometry, especially at sites of dislocations in the skyrmion lattice. Our findings provide a detailed understanding of the elasticity of topologically protected skyrmions and their correlation with underlying material defects.

Enhanced magnetocrystalline anisotropy of Fe30Co70 nanowires by Cu additives and annealing.

The use of 3d transition metal-based magnetic nanowires (NWs) for permanent magnet applications requires large magnetocrystalline anisotropy energy (MAE), which in combination with the NWs' magnetic shape anisotropy yields magnetic hardening and an enhancement of the magnetic energy product. Here, we report on the significant increase in MAE by 125 kJ m(-3) in Fe30Co70 NWs with diameters of 20-150 nm embedded in anodic aluminum oxide templates by adding 5 at.% Cu and subsequent annealing at 900 K. Ferromagnetic resonance (FMR) reveals that this enhancement of MAE is twice as large as the enhancement of MAE in annealed, but undoped NWs. X-ray diffraction (XRD) analysis suggests that upon annealing the immiscible Cu in FeCo NWs causes a crystal reorientation with respect to the NW axis with a considerable distortion of the bcc FeCo lattice. This strain is most likely the origin of the strongly enhanced MAE.

Magnetic hardening of Fe30Co70 nanowires.

3d transition metal-based magnetic nanowires (NWs) are currently considered as potential candidates for alternative rare-earth-free alloys as novel permanent magnets. Here, we report on the magnetic hardening of Fe30Co70 nanowires in anodic aluminium oxide templates with diameters of 20 nm and 40 nm (length 6 µm and 7.5 µm, respectively) by means of magnetic pinning at the tips of the NWs. We observe that a 3-4 nm naturally formed ferrimagnetic FeCo oxide layer covering the tip of the FeCo NW increases the coercive field by 20%, indicating that domain wall nucleation starts at the tip of the magnetic NW. Ferromagnetic resonance (FMR) measurements were used to quantify the magnetic uniaxial anisotropy energy of the samples. Micromagnetic simulations support our experimental findings, showing that the increase of the coercive field can be achieved by controlling domain wall nucleation using magnetic materials with antiferromagnetic exchange coupling, i.e. antiferromagnets or ferrimagnets, as a capping layer at the nanowire tips.

Room-temperature ferromagnetism in antiferromagnetic cobalt oxide nanooctahedra.

Cobalt oxide octahedra were synthesized by thermal decomposition. Each octahedron-shaped nanoparticle consists of an antiferromagnetic CoO core enclosed by eight {111} facets interfaced to a thin (∼ 4 nm) surface layer of strained Co3O4. The nearly perfectly octahedral shaped particles with 20, 40, and 85 nm edge length show a weak room-temperature ferromagnetism that can be attributed to ferromagnetic correlations appearing due to strained lattice configurations at the CoO/Co3O4 interface.

Hollow and yolk-shell iron oxide nanostructures on few-layer graphene in Li-ion batteries.

We report a simple and template-free strategy for the synthesis of hollow and yolk-shell iron oxide (FeOx) nanostructures sandwiched between few-layer graphene (FLG) sheets. The morphology and microstructure of this material are characterized in detail by X-ray diffraction, X-ray absorption near-edge structure, X-ray photoelectron spectroscopy, Raman spectroscopy, scanning and transmission electron microscopy. Its properties are evaluated as negative electrode material for Li-ion batteries and compared with those of solid FeOx/FLG and two commercial iron oxides. In all cases, the content of carbon in the electrode has a great influence on the performance. The use of pristine FLG improves the capacity retention and further enhancement is achieved with the hollow structure. For a low carbon loading of 18 wt. %, the presence of metallic iron in the hollow and yolk-shell FeOx/FLG composite significantly enhances the capacity retention, albeit with a relatively lower initial reversible capacity, retaining above 97% after 120 cycles at 1000 mA g(-1) in the voltage range of 0.1-3.0 V.

Effect of a side reaction involving structural changes of the surfactants on the shape control of cobalt nanoparticles.

Cobalt nanoparticles with different sizes and morphologies including spheres, rods, disks, and hexagonal prisms have been synthesized through the decomposition of the olefinic precursor [Co(η(3)-C8H13)(η(4)-C8H12)] under dihydrogen, in the presence of hexadecylamine and different rhodamine derivatives, or aromatic carboxylic acids. UV-vis spectroscopy, X-ray diffraction, low and high resolution transmission electron microscopy, and electron tomography have been used to characterize the nanomaterials. Especially, the Co nanodisks formed present characteristics that make them ideal nanocrystals for applications such as magnetic data storage. Focusing on their growth process, we have evidenced that a reaction between hexadecylamine and rhodamine B occurs during the formation of these Co nanodisks. This reaction limits the amount of free acid and amine, usually at the origin of the formation of single crystal Co rods and wires, in the growth medium of the nanocrystals. As a consequence, a growth mechanism based on the structure of the preformed seeds rather than oriented attachment or template assisted growth is postulated to explain the formation of the nanodisks.

Bolometer detection of magnetic resonances in nanoscaled objects.

We report on a nanoscaled thermocouple (ThC) as a temperature sensor of a highly sensitive bolometer for probing the dissipative damping of spin dynamics in nanosized Permalloy (Py) stripes. The Au-Pd ThC based device is fabricated by standard electron beam lithography on a 200 nm silicon nitride membrane to minimize heat dissipation through the substrate. We show that this thermal sensor allows not only measurements of the temperature change on the order of a few mK due to the uniform resonant microwave (MW) absorption by the Py stripe but also detection of standing spin waves of different mode numbers. Using a 3D finite element method, we estimate the absorbed MW power by the stripe in resonance and prove the necessity of using substrates with an extremely low heat dissipation like a silicon nitride membrane for successful thermal detection. The voltage responsivity and the noise equivalent power for the ThC-based bolometer are equal to 15 V W(-1) and 3 nW Hz(-1/2), respectively. The ThC device offers a magnetic resonance response of 1 nV/(µ(B) W) corresponding to a sensitivity of 10(9) spins and a temperature resolution of 300 µK under vacuum conditions.

Tunable emission properties by ferromagnetic coupling Mn(II) aggregates in Mn-doped CdS microbelts/nanowires.

Tunable optical emission properties from ferromagnetic semiconductors have not been well identified yet. In this work, high-quality Mn(II)-doped CdS nanowires and micrometer belts were prepared using a controlled chemical vapor deposition technique. The Mn doping could be controlled with time, precursor concentration and temperature. These wires or belts can produce both tunable redshifted emissions and ferromagnetic responses simultaneously upon doping. The strong emission bands at 572, 651, 693, 712, 745, 768, 787 and 803 nm, due to the Mn(II) (4)T1((4)G)  → (6)A1((6)s) d-d transition, can be detected and accounted for by the aggregation of Mn ions at Cd sites in the CdS lattice at high temperature. These aggregates with ferromagnetism and shifted luminescence are related to the excitonic magnetic polaron (EMP) and localized EMP formations; this is verified by ab initio calculations. The correlation between aggregation-dependent optical emissions and ferromagnetic responses not only presents a new size effect for diluted magnetic semiconductors (DMSs), but also supplies a possible way to study or modulate the ferromagnetic properties of a DMS and to fabricate spin-related photonic devices in the future.

Single-step synthesis of monolithic comb-like CdS nanostructures with tunable waveguide properties.

Using a simple in situ seeding chemical vapor deposition (CVD) process, comb-like (branched) monolithic CdS micro/nanostructures were grown. Efficient optical coupling between the backbone and the teeth of the branched architecture is demonstrated by distributing light from an UV-laser-excited spot at one end of the backbone to all branch tips. By varying the deposition conditions, the orientation of the branches with respect to the backbone, their size and density can be tuned as well as the size of the backbone. This in situ seeding CVD method has the potential for a low-cost single-step fabrication of high-quality, micro/nanointegrated photonic devices, with tunable complex waveguiding possibilities.

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 magnetic hysteresis of individual 18 nm Fe nanocubes.

Correlating the electronic structure and magnetic response with the morphology and crystal structure of the same single ferromagnetic nanoparticle has been up to now an unresolved challenge. Here, we present measurements of the element-specific electronic structure and magnetic response as a function of magnetic field amplitude and orientation for chemically synthesized single Fe nanocubes with 18 nm edge length. Magnetic states and interactions of monomers, dimers, and trimers are analyzed by X-ray photoemission electron microscopy for different particle arrangements. The element-specific electronic structure can be probed and correlated with the changes of magnetic properties. This approach opens new possibilities for a deeper understanding of the collective response of magnetic nanohybrids in multifunctional materials and in nanomagnetic colloidal suspensions used in biomedical and engineering technologies.

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).

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.

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.

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.

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.