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Reactive single-step hot-pressing at 1473 K and 35 MPa for 4 h produces dense, bulk, near single-phase, low-cost, and low-criticality Fe2Al1.15B2 and Fe2Al1.1B2Ge0.05Ga0.05 MAB samples, showing second-order magnetic phase transition with favorable magnetocaloric properties around room temperature. The magnetic as well as the magnetocaloric properties can be tailored upon Ge and Ga doping, leading to an increase in the Curie temperature T C and the spontaneous magnetization m S. The maximum isothermal entropy change Δ s T , m a x of hot-pressed Fe2Al1.15B2 in magnetic field changes of 2 and 5 T amounts to 2.5 and 5 J(kgK)−1 at 287.5 K and increases by Ge and Ga addition to 3.1 and 6.2 J(kgK)−1 at 306.5 K, respectively. The directly measured maximum adiabatic temperature change Δ T a d , m a x is improved by composition modification from 0.9 to 1.1 K in magnetic field changes of 1.93 T. Overall, we demonstrate that hot-pressing provides a much faster, more scalable, and processing costs reducing alternative compared to conventional synthesis routes to produce heat exchangers for magnetic cooling devices. Therefore, our criticality assessment shows that hot-pressed Fe-based MAB phases provide a promising compromise of material and processing costs, criticality, and magnetocaloric performance, demonstrating the potential for low-cost and low-criticality magnetocaloric applications around room temperature. [ABSTRACT FROM AUTHOR]

MAX phases are almost exclusively known as carbides, while nitrides and carbonitrides form a significantly underrepresented subgroup even though they have been shown to possess enhanced properties in comparison to their carbide counterparts. One example is the nitride phase Cr2GaN which exhibits a spin density wave magnetic state below T = 170 K, while the metallic carbide phase Cr2GaC follows the MAX phase-typical Pauli-paramagnetic behavior. To investigate the influence on the materials/functional properties of mixing carbon and nitrogen on the X-site, this study aims to synthesize and comprehensively characterize the hitherto unknown carbonitride phase Cr2GaC1-xNx and compare it to the parent phases. Due to the challenging synthesis of (carbo)nitrides in general, a sol-gel-assisted approach is applied which was recently developed by our group. This process was further improved by using timeefficient microwave heating, leading to a highly phase pure product. STEM-EDX analyses reveal a C/N ratio of roughly 2: 1. Temperature-dependent XRD measurements confirm the literature-known magnetic phase transition of the parent nitride phase Cr2GaN, while the incorporation of carbon suppresses the latter. Nonetheless, magnetic characterization of the phases reveals that the magnetic behavior can be specifically influenced by changing the composition of the X-site, resulting in an increase of the susceptibility by increasing the nitrogen amount. Overall, these findings further substantiate the big potential in nitrogencontaining MAX phases, which will also serve as starting materials for future doping studies, i.e. on the M- and A-site, and as precursors for novel 2D MXenes. [ABSTRACT FROM AUTHOR]

MXenes are two-dimensional transition-metal carbides and nitrides with an attractive combination of physicochemical properties, gaining notable potential in many applications. Currently, MXene synthesis is mainly performed from powder precursors whose purity and grain size define the quality and flake size of 2D sheets, typically not exceeding 2–3 μm. In this work, we successfully synthesize macroscopic nanolayered V2CTz MXenes with lateral dimensions larger than 25 μm from a V2AlC single crystal by exploiting a new strategy based on ion implantation. Ne2+ ion implantation of the single-crystal precursor is applied to introduce defects in the crystal structure of V2AlC, which facilitates chemical etching and drastically reduces the etching time down to 8 h (∼10 times lower as compared to conventional synthesis from powder precursors). The quality and morphology of exfoliated macroscopic MXene multilayers have been comprehensively studied by performing detailed analyses based on different kinds of microscopies and spectroscopies. The obtained macroscopic flakes are ideal objects to study the intrinsic physical properties of V2CTz MXenes and explore their potential application, in particular, as membranes. [ABSTRACT FROM AUTHOR]

In this study, we model the chemical stability in the (Cr1–xFex)2AlC MAX phase system using density functional theory, predicting its phase stability for 0 < x < 0.2. Following the calculations, we have successfully synthesized nanolaminated (Cr1–xFex)2AlC MAX phase thin films with target Fe contents of x = 0.1 and x = 0.2 by pulsed laser deposition using elemental targets on MgO(111) and Al2O3(0001) substrates at 600 °C. Structural investigations by X-ray diffraction and transmission electron microscopy reveal MAX phase epitaxial films on both substrates with a coexisting (Fe,Cr)5Al8 intermetallic secondary phase. Experiments suggest an actual maximum Fe solubility of 3.4 at %, corresponding to (Cr0.932Fe0.068)2AlC, which is the highest Fe doping level achieved so far in volume materials and thin films. Residual Fe is continuously distributed in the (Fe,Cr)5Al8 intermetallic secondary phase. The incorporation of Fe results in the slight reduction of the c lattice parameter, while the a lattice parameter remains unchanged. The nanolaminated (Cr0.932Fe0.068)2AlC thin films show a metallic behavior and can serve as promising candidates for highly conductive coatings. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The Cr2AlC MAX phase is a promising parent compound to introduce magnetism to nano-laminated ternary carbides by doping with Mn. Here, we demonstrate that Mn doping of bulk Cr2AlC powder synthesized by arc melting results in incorporation up to 16 at% Mn in the M-layers of the MAX phase. Simultaneously, the relative amount of secondary phases is overall low, however, increases with Mn doping. We successfully applied chemical treatment in dilute hydrochloric acid to eliminate secondary phases and studied the magnetic properties before and after treatment by magnetometry between 3 K and 800 K. All MAX-phases show a paramagnetic response. [ABSTRACT FROM AUTHOR]

FeAl films around equiatomic composition are grown on a-cut (1120) sapphire substrates by ion beam assisted deposition (IBAD) and pulsed laser deposition (PLD) at ambient temperature. Subsequent successive annealing is used to establish chemical order and crystallographic orientation of the films with respect to the substrate. We find a strongly [110]-textured growth for both deposition techniques. Pole figures prove the successful preparation of high quality epitaxial films by PLD with a single in-plane orientation. IBAD-grown films, however, exhibit three in-plane orientations, all of them with broad angular distributions. The difference of the two growth modes is attributed to the existence of a metastable intermediate crystalline orientation as concluded from nonassisted sputter depositions at different substrate temperatures. The formation of the chemically ordered crystalline B2 phase is accompanied by the expected transition from ferromagnetic to paramagnetic behavior of the films. In accordance with the different thermally induced structural recovery, we find a step-like magnetic transition to paramagnetic behavior after annealing for 1 h at TA = 300 °C for IBAD deposition, while PLD-grown films show a gradual decrease of ferromagnetic signals with rising annealing temperatures. [ABSTRACT FROM AUTHOR]

Since its first emergence in 2004, the high‐entropy alloy (HEA) concept has aimed at stabilizing single‐ or dual‐phase multi‐element solid solutions through high mixing entropy. Here, this strategy is changed and renders such massive solid solutions metastable, to trigger spinodal decomposition for improving the alloys' magnetic properties. The motivation for starting from a HEA for this approach is to provide the chemical degrees of freedom required to tailor spinodal behavior using multiple components. The key idea is to form Fe‐Co enriched regions which have an expanded volume (relative to unconstrained Fe‐Co), due to coherency constraints imposed by the surrounding HEA matrix. As demonstrated by theory and experiments, this leads to improved magnetic properties of the decomposed alloy relative to the original solid solution matrix. In a prototype magnetic FeCoNiMnCu HEA, it is shown that the modulated structures, achieved by spinodal decomposition, lead to an increase of the Curie temperature by 48% and a simultaneous increase of magnetization by 70% at ambient temperature as compared to the homogenized single‐phase reference alloy. The findings thus open a pathway for the development of advanced functional HEAs. [ABSTRACT FROM AUTHOR]

Antidot lattices are potential candidates to act as bit patterned media for data storage as they are able to trap nanoscale magnetic domains between two adjacent holes. Here, we demonstrate the combination of micromagnetic modeling and x-ray microscopy. Detailed simulation of these systems can only be achieved by micromagnetic modeling that takes thermal effects into account. For this purpose, a Landau–Lifshitz–Bloch approach is used here. The calculated melting of magnetic domains within the antidot lattice is reproduced experimentally by x-ray microscopy. Furthermore, we compare conventional scanning transmission x-ray microscopy with resolution enhanced ptychography. Hence, we achieve a resolution of 13 nm. The results demonstrate that ptychographic imaging can also recover magnetic contrast in the presence of a strong topological variation and is generally applicable toward magnetic samples requiring ultimate resolution. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The direct and parameter-free measurement of anisotropic electrical resistivity of a magnetic Mn+1AXn (MAX) phase film is presented. A multitip scanning tunneling microscope is used to carry out 4-probe transport measurements with variable probe spacing s. The observation of the crossover from the 3D regime for small s to the 2D regime for large s enables the determination of both in-plane and perpendicular-to-plane resistivities ρab and ρc. A (Cr0.5Mn0.5)2GaC MAX phase film shows a large anisotropy ratio ρ c / ρ ab = 525 ± 49. This is a consequence of the complex bonding scheme of MAX phases with covalent M–X and metallic M–M bonds in the MX planes and predominately covalent, but weaker bonds between the MX and A planes. [ABSTRACT FROM AUTHOR]

MAX phases are typically prepared by high-temperature (oftentimes high-pressure) solid-state methods. Here, we report a new wet chemistry based synthesis technique starting from an aqueous solution of metal nitrates and citric acid to prepare MAX phase Cr2GaC. This solution-processable precursor mixture has the potential to be easily scaled, painted, printed or fabricated onto supports – an advantage that is demonstrated by the formation of hollow carbon microspheres which are decorated with Cr2GaC particles. A small amount of chromium carbide and oxide remains in the product, however, the amount of the latter can be reduced by a larger excess in citric acid in the precursor gel. The transformation mechanism of the initial amorphous gel into highly crystalline and anisotropic MAX phase particles is investigated by detailed thermal analysis. Transmission electron microscopy studies are conducted to elucidate the microstructure of the sol–gel-prepared particles as well as the decorated hollow microspheres. From magnetic susceptibility measurements, the density of states at the Fermi level is deduced reflecting the quality of the Pauli paramagnet Cr2GaC. [ABSTRACT FROM AUTHOR]

The thickness dependence and long-term stability of the magnetic properties of epitaxial (Cr0.5Mn0.5)2GaC MAX phase films on MgO (111) were investigated. For 12.5- to 156-nm-thick films, which corresponds to 10-125 c-axis unit cells, samples were found to be phase pure with negligible c-axis lattice strain of less than 10−4 nm even for the thinnest films. No influence of the interface layers on the magnetic anisotropy, the magnetization or the para- to ferromagnetic phase transition was observed. All samples remained stable for more than one year in ambient conditions. The complex temperature- and magnetic field-dependent magnetism of electrically conducting (Cr0.5Mn0.5)2GaC MAX phase films is environmentally robust over one year and independent on interface effects. [ABSTRACT FROM AUTHOR]

Abstract: Nanomaterials are of enormous value for biomedical applications because of their customizable features. However, the material properties of nanomaterials can be altered substantially by interactions with tissue thus making it important to assess them in the specific biological context to understand and tailor their effects. Here, a genetically controlled system is optimized for cellular uptake of superparamagnetic ferritin and subsequent trafficking to lysosomes. High local concentrations of photoabsorbing magnetoferritin give robust contrast in optoacoustic imaging and allow for selective photoablation of cells overexpressing ferritin receptors. Genetically controlled uptake of the biomagnetic nanoparticles also strongly enhances third‐harmonic generation due to the change of refractive index caused by the magnetite–protein interface of ferritins entrapped in lysosomes. Selective uptake of magnetoferritin furthermore enables sensitive detection of receptor‐expressing cells by magnetic resonance imaging, as well as efficient magnetic cell sorting and manipulation. Surprisingly, a substantial increase in the blocking temperature of lysosomally entrapped magnetoferritin is observed, which allows for specific ablation of genetically defined cell populations by local magnetic hyperthermia. The subcellular confinement of superparamagnetic ferritins thus enhances their physical properties to empower genetically controlled interrogation of cellular processes with deep tissue penetration. [ABSTRACT FROM AUTHOR]

Laser ablation in liquids (LAL) has emerged as a versatile approach for the synthesis of alloy particles and oxide nanomaterials. However, complex chemical reactions often take place during synthesis due to inevitable atomization and ionization of the target materials and decomposition/hydrolysis of solvent/solution molecules, making it difficult to understand the particle formation mechanisms. In this paper, a possible route for the formation of FeMn alloy nanoparticles as well as MnO x nanoparticles, -sheets, and -fibers by LAL is presented. The observed structural, compositional, and morphological variations are clarified by transmission electron microscopy (TEM). The studies suggest that a reaction between Mn atoms and Fe ions followed by surface oxidation result in nonstoichiometric synthesis of Fe-rich FeMn@FeMn2O4 core-shell alloy particles. Interestingly, a phase transformation from Mn3O4 to Mn2O3 and finally to Ramsdellite γ-MnO2 is accompanied by a morphology change from nanosheets to nanofibers in gradually increasing oxidizing environments. High-resolution TEM images reveal that the particle-attachment mechanism dominates the growth of different manganese oxides. [ABSTRACT FROM AUTHOR]

An approach to assemble high aspect ratio nanostrands consisting of magnetic nanowires and their incorporation in a polymer with the aim of tailoring transparent FeNi nanostrand–PMMA-composites is presented. These nanostrands are controllable in length (＜600 μm) and width (＜12 μm) via process parameters and have an ultra-high aspect ratio (∼160). This rapid and universal method provides flexible and transparent magnetic materials with tunable transparency and magnetic attraction force by adjusting the density of nanoparticles in the composite. These composites can be used as a window coating for shielding radio frequency electromagnetic waves while being transparent in the optical range. [ABSTRACT FROM AUTHOR]

We study the reversal mechanisms in a self-assembled, hexagonally ordered Fe antidot array with a period of 200 nm and an antidot diameter of 100 nm which was prepared by polystyrene nanosphere lithography. Direction-dependent information in such a self-assembled sample is obtained by measuring the anisotropic magnetoresistance (AMR) through constrictions processed by focused ion beam milling in nearest neighbor and next nearest neighbor directions. We show that such an originally integral method can be used to investigate the strong in-plane anisotropy introduced by the antidot lattice. The easy and hard axis reversal mechanisms and corresponding AMR signals are modeled by micromagnetic simulations. Additional in-field magnetic force microscopy studies allow the correlation of microscopic switching to features in the integral AMR. We find that the easy axis of magnetization is connected to a distinct periodic magnetic domain pattern, which can be observed during the whole magnetization reversal. While this process is driven by nucleation and propagation of reversed domains, the hard axis reversal is characterized by a (stepwise) rotation of the magnetization via the antidot lattice’ easy axes. [ABSTRACT FROM AUTHOR]

The magnetic properties of Ni nanoparticles (Ni-NPs) embedded in an antiferromagnetic IrMn matrix were investigated. The Ni-NPs of 8.4 nm mean diameter were synthesized by inert gas aggregation. In a second processing step, the Ni-NPs were in situ embedded in IrMn films or SiOx films under ultrahigh vacuum (UHV) conditions. Findings showed that Ni-NPs embedded in IrMn have an exchange bias field HEB = 821 Oe at 10 K, and 50 Oe at 300 K. The extracted value of the exchange energy density is 0.06 mJ m−2 at 10 K, which is in good accordance with the results from multilayered thin film systems. The Ni-NPs embedded in SiOx did not show exchange bias. As expected for this particle size, they are superparamagnetic at T = 300 K. A direct comparison of the Ni-NPs embedded in IrMn or SiOx reveals an increase of the blocking temperature from 210 K to around 400 K. The coercivity of the Ni-NPs exchange coupled to the IrMn matrix at 10 K is 8 times larger than the value for Ni-NPs embedded in SiOx. We studied time-dependent remanent magnetization at different temperatures. The relaxation behavior is described by a magnetic viscosity model which reflects a rather flat distribution of energy barriers. Furthermore, we investigated the effects of different field cooling processes on the magnetic properties of the embedded Ni-NPs. Exchange bias values fit to model calculations which correlate the contribution of the antiferromagnetic IrMn matrix to its grain size. [ABSTRACT FROM AUTHOR]

A lock-in technique for measurement of thermal conductivity and volumetric heat capacity of thin films is presented. The technique is based on the 3ω approach using electrical generation and detection of oscillatory heat along a thin metal strip. Thin films are deposited onto the backside of commercial silicon nitride membranes, forming a bilayer geometry with distinct thermal parameters. Stepwise comparison to an adapted heat diffusion model delivers these parameters for both layers. Highest sensitivity is found for metallic thin films. [ABSTRACT FROM AUTHOR]

We use non-close packed colloidal lithography to prepare hexagonal magnetic antidot arrays with varying diameters at a period of 205 nm. Smaller antidots are attractive for applications as spin waveguides in magnonics. Larger antidots form a magnetically frustrated system, i.e. Kagome spin-ice, as we prove by magnetic force microscopy. The simple but effective approach successfully extends the limits of top-down lithography previously used to study spin-ice configurations and emergent magnetic monopoles towards smaller structures. [ABSTRACT FROM AUTHOR]

We introduce a simple and effective model of a commercial magnetic thin-film sensor for magnetic force microscopy (MFM), and we test the model employing buried magnetic dipoles. The model can be solved analytically in the half-space in front of the sensor tip, leading to a simple 1/R dependence of the magnetic stray field projected to the symmetry axis. The model resolves the earlier issue as to why the magnetic sensors cannot be described reasonably by a restricted multipole expansion as in the point pole approximation: the point pole model must be extended to incorporate a 'lower-order' pole, which we term 'pseudo-pole'. The near-field dependence (α R-1) turns into the well-known and frequently used dipole behavior (α R-3) if the separation, R, exceeds the height of the sensor. Using magnetic nanoparticles (average diameter 18 nm) embedded in a SiO cover as dipolar point probes, we show that the force gradient-distance curves and magnetic images fit almost perfectly to the proposed model. The easy axis of magnetization of single nanoparticles is successfully deduced from these magnetic images. Our model paves the way for quantitative MFM, at least if the sensor and the sample are independent. [ABSTRACT FROM AUTHOR]