Element-Specific Study of Magnetic Anisotropy and Hardening in SmCo5-xCux Thin Films.

This work investigates the effect of copper substitution on the magnetic properties of SmCo5 thin films synthesized by molecular beam epitaxy. A series of thin films with varying concentrations of Cu were grown under otherwise identical conditions to disentangle structural and compositional effects on the magnetic behavior. The combined experimental and theoretical studies show that Cu substitution at the Co3g sites not only stabilizes the formation of the SmCo5 structure but also enhances magnetic anisotropy and coercivity. Density functional theory calculations indicate that Sm(Co4Cu3g)5 possesses a higher single-ion anisotropy as compared to pure SmCo5. In addition, X-ray magnetic circular dichroism reveals that Cu substitution causes an increasing decoupling of the Sm 4f and Co 3d moments. Scanning transmission electron microscopy confirms predominantly SmCo5 phase formation and reveals nanoscale inhomogeneities in the Cu and Co distribution. Our study based on thin film model systems and advanced characterization as well as modeling reveals novel aspects of the complex interplay of intrinsic and extrinsic contributions to magnetic hysteresis in rare-earth-based magnets, i.e., the combination of increased intrinsic anisotropy due to Cu substitution and the extrinsic effect of inhomogeneous elemental distribution of Cu and Co.

Strain- and field-induced anisotropy in hybrid elastomers with elongated filler nanoparticles.

The implementation of anisotropy to functional materials is a key step towards future smart materials. In this work, we evaluate the influence of preorientation and sample architecture on the strain-induced anisotropy in hybrid elastomers containing covalently attached elongated magnetic filler particles. Accordingly, silica coated spindle-type hematite nanoparticles are incorporated into poly(dimethylsiloxane)-based elastomers, and two types of composite architectures are compared: on the one hand a conventional architecture of filled, covalently crosslinked elastomers, and on the other hybrid elastomers that are crosslinked exclusively by covalent attachment of the polymer chains to the particle surface. By the application of external strain and with magnetic fields, the orientational order of the elongated nanoparticles can be manipulated, and we investigate the interplay between strain, magnetic order, and orientational order of the particles by combining 2D small angle X-ray scattering experiments under strain and fields with Mössbauer spectroscopy under similar conditions, and supplementary angular-dependent magnetization experiments. The converging information is used to quantify the order in these interesting materials, while establishing a direct link between the magnetic properties and the spatial orientation of the embedded magnetic nanoparticles.

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.

Deep-branching evolutionary intermediates reveal structural origins of form I rubisco.

The enzyme rubisco (ribulose-1,5-bisphosphate carboxylase/oxygenase) catalyzes the majority of biological carbon fixation on Earth. Although the vast majority of rubiscos across the tree of life assemble as homo-oligomers, the globally predominant form I enzyme-found in plants, algae, and cyanobacteria-forms a unique hetero-oligomeric complex. The recent discovery of a homo-oligomeric sister group to form I rubisco (named form I') has filled a key gap in our understanding of the enigmatic origins of the form I clade. However, to elucidate the series of molecular events leading to the evolution of form I rubisco, we must examine more distantly related sibling clades to contextualize the molecular features distinguishing form I and form I' rubiscos. Here, we present a comparative structural study retracing the evolutionary history of rubisco that reveals a complex structural trajectory leading to the ultimate hetero-oligomerization of the form I clade. We structurally characterize the oligomeric states of deep-branching form Iα and I'' rubiscos recently discovered from metagenomes, which represent key evolutionary intermediates preceding the form I clade. We further solve the structure of form I'' rubisco, revealing the molecular determinants that likely primed the enzyme core for the transition from a homo-oligomer to a hetero-oligomer. Our findings yield new insight into the evolutionary trajectory underpinning the adoption and entrenchment of the prevalent assembly of form I rubisco, providing additional context when viewing the enzyme family through the broader lens of protein evolution.

Tailoring magnetic anisotropy by graphene-induced selective skyhook effect on 4f-metals.

From macroscopic heavy-duty permanent magnets to nanodevices, the precise control of the magnetic properties in rare-earth metals is crucial for many applications used in our daily life. Therefore, a detailed understanding and manipulation of the 4f-metals' magnetic properties are key to further boosting the functionalization and efficiency of future applications. We present a proof-of-concept approach consisting of a dysprosium-iridium surface alloy in which graphene adsorption allows us to tailor its magnetic properties. By adsorbing graphene onto a long-range ordered two-dimensional dysprosium-iridium surface alloy, the magnetic 4f-metal atoms are selectively lifted from the surface alloy. This selective skyhook effect introduces a giant magnetic anisotropy in dysprosium atoms as a result of manipulating its geometrical structure within the surface alloy. Introducing and proving this concept by our combined theoretical and experimental approach provides an easy and unambiguous understanding of its underlying mechanism. Our study sets the ground for an alternative path on how to modify the crystal field around 4f-atoms and therefore their magnetic anisotropies.

Epitaxy Induced Highly Ordered Sm2Co17-SmCo5 Nanoscale Thin-Film Magnets.

Utilizing the molecular beam epitaxy technique, a nanoscale thin-film magnet of c-axis-oriented Sm2Co17 and SmCo5 phases is stabilized. While typically in the prototype Sm(Co, Fe, Cu, Zr)7.5-8 pinning-type magnets, an ordered nanocomposite is formed by complex thermal treatments, here, a one-step approach to induce controlled phase separation in a binary Sm-Co system is shown. A detailed analysis of the extended X-ray absorption fine structure confirmed the coexistence of Sm2Co17 and SmCo5 phases with 65% Sm2Co17 and 35% SmCo5. The SmCo5 phase is stabilized directly on an Al2O3 substrate up to a thickness of 4 nm followed by a matrix of Sm2Co17 intermixed with SmCo5. This structural transition takes place through coherent atomic layers, as revealed by scanning transmission electron microscopy. Highly crystalline growth of well-aligned Sm2Co17 and SmCo5 phases with coherent interfaces result in strong exchange interaction, leading to enhanced magnetization and magnetic coupling. The arrangement of Sm2Co17 and SmCo5 phases at the nanoscale is reflected in the observed magnetocrystalline anisotropy and coercivity. As next-generation permanent magnets require designing of materials at an atomic level, this work enhances our understanding of self-assembling and functioning of nanophased magnets and contributes to establishing new concepts to engineer the microstructure for beyond state-of-the-art magnets.