Ternary ACd 4 P 3 (A = Na, K) Nanostructures via a Hydride Solution-Phase Route
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36 MATERIALS SCIENCE↗
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Energy-relaxation pathways in finite-sized artificial square-ice structures
The energy-relaxation pathway in artificial spin ice structures refers to the series of individual moment reorientations the system undergoes as it relaxes from an initial state to a final low-energy state. The probability of the artificial spin ice structure reaching a ground state depends on the energy of the intermediate states as approximated by an Arrhenius-type relation. In this work, we report that by modifying the geometry of artificial square-ice structures, we can influence the probability of observing the ground state in different configurations. Furthermore, our findings are supported by dipolar energy calculations for various energy-relaxation pathways and the corresponding experimental data obtained by magnetic force microscopy.
Analog computation↗
Effect of Mg Content in Melt-Spun Mn–Bi–Mg–Sb–In Alloys on the Structure and Properties of Field-Annealed Magnets
Mn-Bi alloys modified with Mg and other elements were recently developed into promising rare-earth-free permanent magnets through successive melt-spinning, warm compaction, and short magnetic-field annealing. This letter reports herein on the crystal structures, texture, and magnetic properties observed in Mn 50 Bi 49-x Mg x Sb 0.5 In 0.5 alloys (x = 0, 1.5, 3.0, 4.5) throughout these processing steps. The Mg substitution favors MnBi-based intermetallic phases over the Bi- and Mn-based solid solutions and the stable α intermetallic phase over the metastable β' intermetallic phase. Magnesium increases the c/a ratio of the α phase lattice parameters for all studied x values and it increases the degree of the field-annealing-induced texture for x ≤ 3. The effect of Mg on coercivity is explained as combination of a positive one via the α phase magnetocrystalline anisotropy and a negative one via the development of texture. The effect of the substitution on the maximum energy product additionally involves the decreasing density of the alloys; the optimum x is found to be ≈3. Additionally reported are the thermal properties of selected alloys. The mechanism of field-annealing effect on the coercivity is briefly discussed.
36 MATERIALS SCIENCE↗
Development of high B s Fe–Ni-based metal amorphous nanocomposite by optimization of glass-forming ability
Thermocalc simulations identified compositions with good glass-forming ability (GFA) by locating minima in liquidus temperature, and solidification range in (Fe 70 Ni 30 ) x (B-Si-Nb) 100-x alloys with x = 82% and x = 85%, increased compared to previously developed x = 80% alloys. 3 compositions in the x = 82% system and 1 in the x = 85% system were successfully cast as amorphous magnetic ribbon. Magnetic properties of as-cast alloys showed improvements in Curie temperature and saturation induction, especially for the 85% alloy. Crystallization behavior in the 85% alloy was determined to occur as a 2-step process. Annealing studies showed (Fe 70 Ni 30 ) 82 Nb 2 Si 0 B 16 and (Fe 70 Ni 30 ) 82 Nb 3 Si 0 B 15 alloys to exhibit low coercivity and high B s with annealing. TEM results show significant crystallization in as-cast ribbon. The (Fe 70 Ni 30 ) 85 Nb 0.5 Si 0 B 14.5 alloy as-cast has small, uniformly distributed grains, allowing a useful nanocrystalline alloy to be produced as cast. Lastly, the parameter ΔT xg , the temperature range in which the material can be thermomechanically processed, was in the range of 12–23 °C.
36 MATERIALS SCIENCE↗
Synthesis and behavior of bulk iron nitride soft magnets via high-pressure spark plasma sintering
Abstract In this study, dense bulk iron nitrides (Fe x N) were synthesized for the first time ever using spark plasma sintering (SPS) of Fe x N powders. The Fe 4 N phase of iron nitride in particular has significant potential to serve as a new soft magnetic material in both transformer and inductor cores and electrical machines. The density of SPSed Fe x N increased with SPS temperature and pressure. The microstructure of the consolidated bulk Fe x N was characterized with X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), and superconducting quantum interference device (SQUID) magnetometry. XRD revealed a primary phase of Fe 4 N with secondary phases of Fe 3 N and metallic iron. Finite element analysis (FEA) was also applied to investigate and explain localized heating and temperature distribution during SPS. The effects of processing on interface bonding formation and phase evolution were investigated and discussed in detail to provide insight into fundamental phenomena and microstructural evolution in SPSed Fe x N. Graphic abstract
36 MATERIALS SCIENCE↗
Magnetic skyrmion diode: Unidirectional skyrmion motion via symmetry breaking of potential energy barriers
In this work, we realize a magnetic skyrmion diode operated by a unidirectional skyrmion transport that flows in only one direction, which is highly significant for information processing in spintronic and nanoelectronic devices. We easily control the skyrmion transport by engineering asymmetric shapes of geometric structures. Here, we present a simple method to describe the underlying mechanism behind the unidirectional skyrmion transport by characterizing the topography of potential energy surfaces from a purely geometric perspective. Our approach enables a deeper physical insight into skyrmion transport manipulation and efficient design of skyrmion-based devices in geometric structures.
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Iron-assisted growth of anisotropic ZnO nanostructures
Anisotropic nanostructures offer a promising pathway to modulate structure-function relationships of materials. However, the correlation between growth direction of high-quality anisotropic nanostructures, the synthesis conditions and mechanisms controlling their growth, and their magnetic and optical properties remain underexplored. In this study, we developed an iron-assisted anisotropic growth method to form zinc oxide nanostructures on the O-polar (0001̄) surface, resulting in two distinct ZnO-based nanostructures: hand-shaped nanostructures and truncated hexagonal nanopyramids. In contrast to most reports of anisotropic nanostructure synthesis, which primarily focus on morphology control through ligand-ligand interactions, the current study probes the effects of doping on anisotropic growth, and how doping, along with ligand-ligand interactions and facet-specific ligand binding, control nanostructure morphology. The reaction mechanisms leading to formation of these novel structures were thoroughly probed by systematically manipulating synthesis parameters. A two-step formation mechanism was identified: first, a hexagonal platform forms through an initial homogeneous nucleation process, followed by secondary heterogeneous nucleation, which results in metastable secondary nanostructures growing on the oxygen-rich template. Optical and magnetic properties of these Fe/ZnO nanostructures were characterized. Our findings provide a new strategy that uses a magnetic element as a dopant to build new nanostructures of ZnO with controllable size and shape growing on an oxygen-rich crystal plane. These materials could have applications in novel technologies where both optoelectronic and magnetic properties are of interest.
Xuan, Zhengxi↗
Nanostructure refinement and phase formation of flash annealed FeNi-based soft magnetic alloys
In this work, the resulting nanocomposite microstructures of FeNi nanocrystallites under different heating and cooling rates (5 °C/min vs 400-500 °C/s) is investigated. Conventional furnace annealing under low heating rates and slow cooling resulted in both BCC α-FeNi and FCC γ-FeNi nanocrystallites with an average grain size on the order of 25-27 nm whereas high heating rates achieved via flash annealing techniques have enabled a dramatically refined microstructure consisting of 5-7 nm grains with FCC γ-FeNi phase and found to be the dominant phase following primary crystallization. Grain size refinement and phase identity optimization yielded low values of coercivities-17 A/m and high permeability similar to 11 x 10 3 measured at 400 Hz/1 kA/m in flash annealed samples at 450 °C for 5 s. The magnetic behavior and the underlying mechanism of optimal soft magnetic properties are discussed in terms of the critical role of the grain size in domain wall pinning and coercivity.
36 MATERIALS SCIENCE↗
Formation of Complex Spin Textures in Thermally Demagnetized La 0.7 Sr 0.3 Mn O 3 Artificial-Spin-Ice Structures
Artificial spin ices (ASIs) have traditionally been designed such that each nanomagnet possesses a single-domain magnetic configuration that is assumed to be minimally perturbed by interisland dipolar interactions. Using x-ray photoemission electron microscopy to perform magnetic domain imaging, we study thermally demagnetized La 0.7 Sr 0.3 MnO 3 -based brickwork ASI arrays and showed that complex spin textures (CSTs) can be stabilized through an appropriate selection of nanoisland width and interisland spacing. While the width dependence can be explained through the dominance of shape anisotropy in isolated nanoislands, the ASIs we investigate demonstrate a complex dependence on both the nanoisland width and interisland spacing. Micromagnetic simulations reveal that interisland dipolar interactions play a role in the formation of CSTs, which are composed of single- and double-vortex states. Furthermore, energy analysis of the simulations provides an understanding of the system energetics that arises from a delicate balance between intraisland effects (i.e., shape anisotropy and exchange energy) and interisland effects (i.e., dipolar interactions between nearest-neighbor nanoislands).
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
Extreme-ultraviolet spatiotemporal vortices via high harmonic generation
Spatiotemporal optical vortices (STOVs) are space–time structured light pulses with a unique topology that couples spatial and temporal domains and carry transverse orbital angular momentum (OAM). Up to now, their generation has been limited to the visible and infrared regions of the spectrum. During the last decade, it was shown that through the process of high-order harmonic generation, it is possible to upconvert spatial optical vortices that carry longitudinal OAM from the near-infrared into the extreme-ultraviolet (EUV), thereby producing vortices with distinct femtosecond and attosecond structure. In this work, we demonstrate theoretically and experimentally the generation of EUV spatiotemporal and spatiospectral vortices using near-infrared STOV driving laser pulses. Here, we use analytical expressions for focused STOVs to perform macroscopic calculations of high-order harmonic generation that are directly compared to the experimental results. As STOV beams are not eigenmodes of propagation, we characterize the highly charged EUV STOVs in both the near and far fields to show that they represent conjugated spatiotemporal and spatiospectral vortex pairs. Our work provides high-frequency light beams topologically coupled at the nanometre/attosecond scales domains with transverse OAM that could be suitable to explore electronic dynamics in magnetic materials, chiral media and nanostructures.
High-harmonic generation↗
Tailoring the Magnetic and Hyperthermic Properties of Biphase Iron Oxide Nanocubes through Post-Annealing
Tailoring the magnetic properties of iron oxide nanosystems is essential to expanding their biomedical applications. In this study, 34 nm iron oxide nanocubes with two phases consisting of Fe3O4 and α-Fe2O3 were annealed for 2 h in the presence of O2, N2, He, and Ar to tune the respective phase volume fractions and control their magnetic properties. X-ray diffraction and magnetic measurements were carried out post-treatment to evaluate changes in the treated samples compared to the as-prepared samples, showing an enhancement of the α-Fe2O3 phase in the samples annealed with O2 while the others indicated a Fe3O4 enhancement. Furthermore, the latter samples indicated enhancements in crystallinity and saturation magnetization, while coercivity enhancements were the most significant in samples annealed with O2, resulting in the highest specific absorption rates (of up to 1000 W/g) in all the applied fields of 800, 600, and 400 Oe in agar during magnetic hyperthermia measurements. The general enhancement of the specific absorption rate post-annealing underscores the importance of the annealing atmosphere in the enhancement of the magnetic and structural properties of nanostructures.
Crystallography↗
Vertically Aligned Single-Crystalline CoFe 2 O 4 Nanobrush Architectures with High Magnetization and Tailored Magnetic Anisotropy
Micrometer-tall vertically aligned single-crystalline CoFe 2 O 4 nanobrush architectures with extraordinarily large aspect ratio have been achieved by the precise control of a kinetic and thermodynamic non-equilibrium pulsed laser epitaxy process. Direct observations by scanning transmission electron microscopy reveal that the nanobrush crystal is mostly defect-free by nature, and epitaxially connected to the substrate through a continuous 2D interface layer. In contrast, periodic dislocations and lattice defects such as anti-phase boundaries and twin boundaries are frequently observed in the 2D interface layer, suggesting that interface misfit strain relaxation under a non-equilibrium growth condition plays a critical role in the self-assembly of such artificial architectures. Further, magnetic property measurements have found that the nanobrushes exhibit a saturation magnetization value of 6.16 μB/f.u., which is much higher than the bulk value. The discovery not only enables insights into an effective route for fabricating unconventional high-quality nanostructures, but also demonstrates a novel magnetic architecture with potential applications in nanomagnetic devices.
36 MATERIALS SCIENCE↗
Magnetic and Optical Properties of Au–Co Solid Solution and Phase-Separated Thin Films and Nanoparticles
The chemical composition and morphology of Au x Co 1–x thin films and nanoparticles are controlled via a combination of cosputtering, pulsed laser-induced dewetting (PLiD), and annealing, leading to tunable magnetic and optical properties. Regardless of chemical composition, the as-deposited thin films and as-PLiD nanoparticles are found to possess a face-centered cubic (FCC) Au x Co 1–x solid-solution crystal structure. Annealing results in large phase-separated grains of Au and Co in both the thin films and nanostructures for all chemical compositions. The magnetic and optical properties are characterized via vibrating sample magnetometry (VSM), ellipsometry, optical transmission spectroscopy, and electron energy loss spectroscopy (EELS). Despite the exceptionally high magnetic anisotropy inherent to Co, the presence of sufficient Au (72 atom %) in the Au x Co 1–x solid solution results in superparamagnetic thin films. Among the as-PLiD nanoparticle samples, an increased Co composition leads to a departure from traditional ferromagnetism in favor of wasp-waisted hysteresis caused by magnetic vortices. Phase separation resulting from annealing leads to ferromagnetism for all compositions in both the thin films and nanoparticles. The optical properties of Au x Co 1–x nanostructures are also largely influenced by the chemical morphology, where the Au x Co 1–x intermixed solid solution has significantly damped plasmonic performance relative to pure Au and comparable to pure Co. Phase separation greatly enhances the quality factor, optical absorption, and electron energy loss spectroscopy (EELS) signatures. The enhancement of the localized surface plasmon resonances (LSPRs) scales with the reduction in Co composition, despite EELS evidence that excitation of the Co portions of a nanoparticle can provide a similar, and in some instances enhanced, LSPR resonance compared to Au. This behavior, however, is seemingly limited to the LSPR dipole mode, while higher-order modes are greatly damped by a Co aloof position. As a result, this observed magneto-plasmonic functionality and tunability could be applicable in biomedicine, namely, cancer therapeutics.
annealing (metallurgy)↗
Nanomaterials and Sustainability
Nanostructuring adds a tremendous degree of tunability to the optical, electronic, magnetic, tribological, and chemical properties of matter. As a result, nanostructured materials already play major roles in the many technologies and industries that provide the comfort and convenience of our everyday lives. Although there are examples of nanostructured materials that currently enhance sustainable technologies, such as for batteries and electrolyzers, the potential impact of nanoscale materials on sustainability has likely not nearly been realized when one considers that the nanostructure–property–composition exploration phase space is almost infinite. We can find inspiration from nature, which builds and assembles nanostructured materials into hierarchical biological structures to perform the enormously complex functions of life, all the while doing so with a relatively small set of elements that are sustainably sourced. This contrasts with current technology, where performance demands often require a greater and greater diversity of elements from the periodic table, some of which are very challenging to be sustainably sourced or recycled.
77 NANOSCIENCE AND NANOTECHNOLOGY↗
Isotropic nanocrystalline Sm(Fe,Co) 11.3 Ti 0.7 magnets modified with B and Zr
Rare-earth-lean Sm(Fe,Co,Ti) 12 alloys with the ThMn 12 crystal structure and less than one Ti atom per formula unit have the potential of exceptionally powerful permanent magnets, but all prior attempts to develop high coercivity in bulk alloys, especially coercivity combined with crystallographic texture, have fallen short of the expectations. This study was aimed at improvement of the currently best Sm(Fe,Co,Ti) 12 magnets prepared through melt-spinning which are inherently isotropic. Modifications of the alloys with B and Zr, already demonstrated in earlier studies to be effective separately, have been implemented simultaneously. Here, a systematic study of Sm 1.1-x (Fe,Co) 11.3-y Ti 0.7 B y alloys melt-spun at a tangential speed of 50 m/s and annealed at 600–950 °C allowed for monitoring the continuous evolution of the two consecutive crystal structures, those of the TbCu 7 and ThMn 12 types. Zirconium was found to facilitate the formation of the 1:12 structure at the expense of the 1:7, whereas boron has the opposite effect, at certain concentrations completely suppressing the 1:12. When the two alloying elements are introduced simultaneously, they inhibit growth of the 1:12 crystallites at annealing temperatures higher than 800 °C, thus allowing for the development of a higher coercivity. Because of instrumental limitations, bulk magnets were prepared through a two-step process – compaction of the melt-spun ribbons at 650 °C and additional treatment at a higher temperature – and they were characterized by a reduced, 90–93%, density. Nevertheless, an isotropic Sm 0.9 Zr 0.2 (Fe,Co) 10.8 Ti 0.7 B 0.5 magnet exhibited fair values of the remanence (7.4 kG), maximum energy product (8.5 MGOe) and coercivity (5.4 kOe), as well as high Curie temperature of 525 °C and remarkably small temperature coefficient of the coercivity, -0.25%/°C.
36 MATERIALS SCIENCE↗
Atomistic theories and Simulations of Multiferroics
The goal of this award was to build a research program aimed at investigating puzzling complex phenomena in multiferroics, that are systems possessing electric and magnetic dipoles. We first emphasized the study of multiferroic nanostructures, that are 0D, 1D, 2D systems as well as superlattices and then also study multiferroics as a whole, i.e., bulks as well. In order to fully understand such complex systems, we also decided to study magnetic systems and ferroelectrics, both in their nanostructure and bulk forms. For that and in addition to use standard Density Functional Theory codes, we developed and used ab-initio tools that are able to model properties of large supercells (about a million atoms nowadays) at finite temperature and for any mechanical and boundary conditions. We also collaborated with experimentalists to fully understand the systems under study. The whole program resulted in 108 publications that are listed at the end of this report. In the following, I will put an emphasis on some publications before the last award period and also indicate a description of the last award period.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Functional soft materials and methods of making and using thereof
Disclosed are functional materials for use in additive manufacturing (AM). The functional material can comprise an elastomeric composition (e.g., a silicone composite) for use in, for example, direct ink writing. The elastomeric composition can include and elastomeric resin, and a magnetic nanorod filler dispersed within the elastomeric resin. Nanorod characteristics (e.g., length, diameter, aspect ratio) can be selected to create 3D-printed constructs with desired mechanical properties along different axes. Furthermore, since nickel nanorods are ferromagnetic, the spatial distribution and orientation of nanorods within the continuous phase can be controlled with an external magnetic field. This level of control over the nanostructure of the material system offers another degree of freedom in the design of functional parts and components with anisotropic properties. Magnetic fields can be used to remotely sense compression of the constructs, or alternatively, control the stiffness of these materials.
Berkland, Cory↗
Functional soft materials and methods of making and using thereof
Disclosed are functional materials for use in additive manufacturing (AM). The functional material can comprise an elastomeric composition (e.g., a silicone composite) for use in, for example, direct ink writing. The elastomeric composition can include an elastomeric resin, and a magnetic nanorod filler dispersed within the elastomeric resin. Nanorod characteristics (e.g., length, diameter, aspect ratio) can be selected to create 3D-printed constructs with desired mechanical properties along different axes. Furthermore, since nickel nanorods are ferromagnetic, the spatial distribution and orientation of nanorods within the continuous phase can be controlled with an external magnetic field. This level of control over the nanostructure of the material system offers another degree of freedom in the design of functional parts and components with anisotropic properties. Magnetic fields can be used to remotely sense compression of the constructs, or alternatively, control the stiffness of these materials.
Berkland, Cory↗