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Enhancing stability, magnetic anisotropy, and coercivity of manganese aluminum: Machine learning, ab initio , and micromagnetic modeling
The binary manganese aluminum (MnAl) alloy with L1 0 crystal structure is a promising rare earth (RE) element-free permanent magnetic material because of its exceptional magnetic properties. However, experimentally synthesizing it in a stable bulk form is extremely challenging. Here, in this study, an alternative method of stabilizing the material, a pathway for experimental synthesis and validation, is proposed and theoretically verified. This is done by partially substituting Mn and Al sites with Fe and Ni and identifying its enhanced phase stability, saturation magnetization density, magnetic anisotropy, and coercivity from density functional theory (DFT), machine learning (ML) crystal graph convolution neural network (CGCNN), and micro-magnetic modeling. When considering a fixed 50% Ni, the magnetic anisotropy increases with the increasing Fe content but decreases the formation energy. The calculated formation energies, elastic constants, and phonon frequencies demonstrate that the binary and quaternary compositions are stable. Most importantly, in 50% Fe and Ni-substituted-equiatomic phase, magnetic anisotropy constants and saturation magnetization density increase by 56% and 23% as compared to the MnAl. Further, the coercivity of the equiatomic phase predicted with micro-magnetic modeling is higher by 17% than the parent compound.
Phonon spectrum of $\mathrm{Pr_2Zr_2O_7}$ and $\mathrm{Pr_2Ir_2O_7}$ as evidence of coupling of the lattice with electronic and magnetic degrees of freedom
Magnetic materials with pyrochlore crystal structure form exotic magnetic states due to the high lattice frustration. Here in this work we follow the effects of coupling of the lattice and electronic and magnetic degrees of freedom in two praseodymium-based pyrochlores $\mathrm{Pr_2Zr_2O_7}$ and $\mathrm{Pr_2Ir_2O_7}$. In either of these materials, the presence of magnetic interactions does not lead to magnetically ordered low temperature states; however, their electronic properties are different. A comparison of Raman phonon spectra of $\mathrm{Pr_2Zr_2O_7}$ and $\mathrm{Pr_2Ir_2O_7}$ allows us to identify magnetoelastic coupling in $\mathrm{Pr_2Zr_2O_7}$ that elucidates its magnetic properties at intermediate temperatures and allows us to characterize phonon-electron scattering in the semimetallic $\mathrm{Pr_2Ir_2O_7}$. We also show that the effects of random disorder on the Raman phonon spectra is small.
Fabrication of magnetic core PEI-silica shell particles
Highlights: • PEI-silica shell fabrication was developed for iron-carbonyl core material. • Magnetic separation of core-free by-product of the fabrication proved successful. • Varying fabrication method/concentration successfully tuned shell characteristics. • Sonication methods produced smooth coatings with a trend towards multicore particles. • Raspberry-like coatings were made by the slow addition, one- and two-pot methods. - Abstract: Magnetic core-silica shell particles combine the physico-chemical properties of the silica shell with the magnetic properties of the core. Seven possible particle coating methods utilizing the biomimetic polyamine polyethyleneimine (PEI) as the silication catalyst, have been identified and the objective of this study was to link the properties of the final PEI-silica coating with the methodology. The PEI-silica coated carbonyl iron particles were characterized via scanning electron microscopy, energy dispersive X-ray spectroscopy and Fourier transfer infrared spectroscopy. Varying the fabrication method and silane concentration successfully tuned the shell characteristics. Methods using sonication produced smooth more evenly distributed coatings with a tendency towards multicore particles. In contrast, raspberry-like coatings were produced via the slow addition, one- and two-pot methods. The magnetic separation process after synthesis achieved a degree of purification that makes these core–shell particles useful for potential applications that require specific surface interactions and the ease of magnetic separation.
High Pressure Synthesis of New Magnets, Featuring Diamagnetic Sources of Anisotropy
Permanent magnets are the functional component of electric motors and generators found in numerous renewable energy applications spanning from regenerative brakes to wind turbines. Magnets that generate higher magnetic flux per volume are central to improved energy generation in these applications. To develop a new class of permanent magnets while retaining the properties conferred by rare-earth elements, a fundamentally different approach is required. We hypothesize that by engendering a covalent interaction between two elements, it will be possible to interact the two components of a magnetic moment—spin and orbital angular momentum—from two separate atoms to form a complete magnetic moment. This seed project focuses on the scale up of the compound FeBi 2 , which was initially synthesized in our laboratory. Scale up approaches include slow decompression, alternate synthetic routes, and using fabrication approaches to more intimately mix the precursor elements. We also pursued the synthesis of new phases in the Mn-Bi system targeted to create new magnetic materials. In our initial experiments we decompressed FeBi 2 down to 2.9 GPa, demonstrating a kinetic stability to the phase that enabled it to be recovered to an order of magnitude lower pressure than that needed to synthesize it (30 GPa). Our goal is to recover this exciting material to ambient pressures so that we can isolate samples for detailed physical properties measurements. We have undertaken three distinct approaches toward that goal, which we summarize below. Our two most notable results are the formation of a quenchable phase through antimony doping of FeBi 2 , and the development of a new approach to preparing samples for diamond anvil cell syntheses.
Magnetically self-assembled SrFe12O19/Fe-Co core/shell particles
Epitaxial growth to synthesize core/shell-structured materials is limited because large lattice mismatches are common between materials. Magnetically hard/soft, core/shell-structured materials can be potentially used for rare-earth free permanent magnets, but their synthesis presents a challenge. We report a wet chemistry method to synthesize core/shell structured particles consisting of a magnetically hard SrFe12O19 core and a soft Fe-Co shell, with a lattice mismatch of similar to 100%, which cannot be achieved by conventional epitaxial growth or other alternative methods. When decreasing the size of the magnetically soft Fe-Co nanoclusters to below 5 nm, we show that they can be magnetically attracted by the hard SrFe12O19 to form core/shell structured particles. An AC demagnetization experiment demonstrates the formation mechanism of the core/shell particles, and their magnetic hysteresis loop shows potential for use as rare-earth free permanent magnets. Published by Elsevier B.V.
Transverse barrier formation by electrical triggering of a metal-to-insulator transition
Application of an electric stimulus to a material with a metal-insulator transition can trigger a large resistance change. Resistive switching from an insulating into a metallic phase, which typically occurs by the formation of a conducting filament parallel to the current flow, is a highly active research topic. Using the magneto-optical Kerr imaging, we found that the opposite type of resistive switching, from a metal into an insulator, occurs in a reciprocal characteristic spatial pattern: the formation of an insulating barrier perpendicular to the driving current. This barrier formation leads to an unusual N-type negative differential resistance in the current-voltage characteristics. We further demonstrate that electrically inducing a transverse barrier enables a unique approach to voltage-controlled magnetism. By triggering the metal-to-insulator resistive switching in a magnetic material, local on/off control of ferromagnetism is achieved using a global voltage bias applied to the whole device.
Vector potential photoelectron microscopy
A new class of electron microscope has been developed for the chemical microanalysis of a wide range of real world samples using photoelectron spectroscopy. Highly structured, three-dimensional samples, such as fiber mats and fracture surfaces can be imaged, as well as insulators and magnetic materials. The new microscope uses the vector potential field from a solenoid magnet as a spatial reference for imaging. A prototype instrument has demonstrated imaging of uncoated silk, magnetic steel wool, and micron-sized single strand tungsten wires.
Superconductive magnets
Superconductive materials and magnet design, discussing stabilization methods
Development and evaluation of magnetic and electrical materials capable of operating in the 800 deg to 1600 deg F temperature range Second quarterly report, Mar. 1 - May 31, 1965
Magnetic materials for high temperature operation, high temperature capacitor feasibility, and bore seal development under space simulated environment
Nanocomposite Magnetic Technology for High Frequency MW Scale Power Conversion
The purpose of this project was to demonstrate the use of advanced magnetic materials in a medium voltage DC-DC converter for photovoltaic applications. The lead, alloy development team met project development milestones targeting a low loss material (<20 W/kg at 10kHzT), alloy resistivity (>150μΩcm amorphous phase resistivity), evaluation of the operational lifetime of the material (continuous operation above 155C), and the performance metric (power ratio >100) for a new class of Co-rich alloys with tunable permeability. Material manufacturability was demonstrated in continuously casting over 5 kg batches of 1’’ width, 18μm thickness (less than 80-120% deviation), amorphous ribbon, and processing including field and strain annealing as well as rolling both Fe and Co based alloys to less the 15μm was achieved. Parallel technology to markets efforts found that while a more compact and more efficient converter, which reduces the balance of plant cost, would enjoy a $0.10/W premium over current technology. Due to uncertainty in future energy policy and barriers to market entry the technology to market analyses recommended partnering with an existing manufacturer. The industrial and transportation electric motor market was also identified as one standing to benefit from this material technology and key personnel within this market were identified. With the assistance of Dynapower the converter prototype was tested to 300 VDC (18 kVA) before the resonant capacitors failed. The prototype incorporated several subsystems including the passive and active components at the engineering scale and exposed at least one weak point in the prototype. Independent testing on the core materials predicts that the core would have met the operating specifications, but this component was not tested at nominal power. Based on this prediction and the demonstrated construction of the prototype core, we recommend that the core material is designated TRL 5. The CMU team is currently working with Eaton to identify opportunities further test cores in inductive components.
Thermoelectricity in transition metal compounds: The role of spin disorder
Here, at room temperature and above, most magnetic materials adopt a spin-disordered (paramagnetic) state whose electronic properties can differ significantly from their low-temperature, spin-ordered counterparts. Yet computational searches for new functional materials usually assume some type of magnetic order. In the present work, we demonstrate a methodology to incorporate spin disorder in computational searches and predict the electronic properties of the paramagnetic phase. We implement this method in a high-throughput framework to assess the potential for thermoelectric performance of 1350 transition-metal sulfides and find that all magnetic systems we identify as promising in the spin-ordered ground state cease to be promising in the paramagnetic phase due to disorder-induced deterioration of the charge carrier transport properties. We also identify promising non-magnetic candidates that do not suffer from these spin disorder effects. In addition to identifying promising materials, our results offer insights into the apparent scarcity of magnetic systems among known thermoelectrics and highlight the importance of including spin disorder in computational searches.
Probing short-range magnetic order in a geometrically frustrated magnet by means of the spin Seebeck effect
The spin Seebeck effect (SSE) is a phenomenon where a spin current is generated from thermal excitations in magnetic materials. It is believed that magnetic long-range order (LRO) is not required for SSE, while short-ranged order (SRO) plays an important role. However, a definitive experimental demonstration of the connection between the SSE and SRO has been missing. Here, we show that the SSE is able to probe a specific SRO in a model geometrically frustrated magnet Gd 3 Ga 5 O 12 (GGG). A field-induced SRO in GGG is detected by the SSE in the temperature range 2-5 K. The origin of the SRO is verified by comparing the SSE data directly to existing neutron scattering measurements at much lower temperatures (T < 0.9 K), where field-induced LRO exists. Our theoretical calculations of the magnetic structure further confirm the anisotropic field dependence of the SRO in GGG. Furthermore, these findings establish that the SSE can serve as an effective probe of SRO in geometrically frustrated magnets.
Effect of Surface Oxidation and Crystal Thickness on the Magnetic Properties and Magnetic Domain Structures of Cr 2 Ge 2 Te 6
van der Waals (vdW) magnetic materials, such as Cr 2 Ge 2 Te 6 (CGT), show promise for memory and logic applications. This is due to their broadly tunable magnetic properties and the presence of topological magnetic features such as skyrmionic bubbles. A systematic study of thickness and oxidation effects on magnetic domain structures is important for designing devices and vdW heterostructures for practical applications. Here, we investigate thickness effects on magnetic properties, magnetic domains, and bubbles in oxidation-controlled CGT crystals. We find that CGT exposed to ambient conditions for 5 days forms an oxide layer approximately 5 nm thick. This oxidation leads to a significant increase in the oxidation state of the Cr ions, indicating a change in local magnetic properties. This is supported by real-space magnetic texture imaging through Lorentz transmission electron microscopy. By comparing the thickness-dependent saturation field of oxidized and pristine crystals, we find that oxidation leads to a nonmagnetic surface layer that is thicker than the oxide layer alone. We also find that the stripe domain width and skyrmionic bubble size are strongly affected by the crystal thickness in pristine crystals. Finally, these findings underscore the impact of thickness and surface oxidation on the properties of CGT, such as saturation field and domain/skyrmionic bubble size, and suggest a pathway for manipulating magnetic properties through a controlled oxidation process.
Machine learning assisted search for Fe–Co–C ternary compounds with high magnetic anisotropy
We employ a machine learning (ML)-guided framework to explore rare earth free magnetic materials, specifically focusing on Fe–Co–C ternary compounds for potential use in permanent magnets. Utilizing a specifically trained crystal graph convolutional neural network model, we efficiently screen a vast space of nearly a million substitutional structures to select 620 promising structures for further investigation by first-principles calculation. We predict five low-energy metastable Fe–Co–C compounds with formation energy less than 150 meV/atom above the convex hull. These compounds exhibit high magnetization (Js > 1.0 T) and significant magnetic anisotropy (K1 > 1.0 MJ/m3), making them promising candidates for permanent magnet applications. The phonon calculations indicate these compounds are dynamically stable. Our ML-guided framework demonstrates the utility of rapidly identifying novel materials with tailored magnetic properties.
Characterizations of maghemite thin films prepared by a sol-gel method
Iron is one of the abundant elements of Mother Nature and its compound, iron oxide is an interesting material to study since its discovery in the form of magnetite. It can exist in many phases such as hematite and maghemite, this unique nature has put it as a potential candidate in various applications. The aim of this work is to study the influence of different precursor concentrations on the microstructural and magnetic properties of iron oxide thin film. All samples were prepared via the sol-gel method followed by a spin coating technique on quartz substrates. Iron oxide films were confirmed as maghemite phase from X-ray diffraction patterns. The film morphology was examined by a field emission scanning electron microscope and it showed non-systematic value of average grain size and film thickness throughout the study. Hysteresis loop further confirmed that maghemite is a magnetic material when it was characterized by a vibrating sample magnetometer. The coercivity did not show any correlation with molarity. Nevertheless, it increased as the precursor concentration of the film increased due to the domain behaviour. In conclusion, maghemite thin films were successfully synthesized by the sol-gel method with different precursor concentrations in this work.
Fractional electrical dimensionality in the spin solid phase of artificial honeycomb lattice
Two-dimensional artificial magnetic honeycomb lattices are at the forefront of research on unconventional magnetic materials. Among the many emergent magnetic phases that are predicted to arise as a function of temperature, the low temperature spin solid phase with zero magnetization and entropy is of special importance. Here, we report an interesting perspective to the consequence of spin solid order in an artificial honeycomb lattice of ultra-small connected elements using electrical dimensionality analysis. At low temperature, T ≤ 30 K, the system exhibits a very strong insulating characteristic. The electrical dimensionality analysis of the experimental data reveals a fractional dimensionality of d = 0.6(0.04) in the spin solid phase of honeycomb lattice at low temperature. The much smaller electrical dimension in the spin solid phase, perhaps, underscores the strong insulating behavior in this system. Furthermore, the fractional dimensionality in an otherwise two-dimensional system suggests a non-surface-like electrical transport at low temperature in an artificial honeycomb lattice.
Interplay between defect transport and cation spin frustration in corundum-structured oxides
Despite the fundamental importance of mass transport, there is still a lack of knowledge regarding the mechanisms in many materials. In particular, how the magnetic spin structure interacts with migrating defects is unclear. In this work, using density functional theory to examine cation interstitial transport in antiferromagnetic corundum-structured oxides, we reveal an interplay between the migration of the interstitial and the magnetic structure of the oxide. The magnetic spin configuration impacts the migration energy of the migrating defect but, critically, the defect modifies the spin configuration. Thus, the two aspects change in concert to modify one another. This has profound implications for mass transport in magnetic materials.