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DOE OSTI2022

3D magnetic imaging using electron vortex beam microscopy

Abstract Electron vortex beams are free-electron waves that carry orbital angular momentum. There has been growing theoretical and experimental interest in the use of electron vortex beams as a tool for the investigation of magnetic materials. However, due to the complex wavefront of the propagating waves, a deeper understanding of the interaction of electron vortex beams and the magnetic sample is needed. Here we calculate the magnetic phase shift that an electron vortex beam obtains upon transmitting through a magnetic sample. We show that this magnetic phase shift is influenced by the out-of-plane magnetization, which is a unique characteristic of incident electron vortex beams and is proportional to their orbital angular momentum. Finally, we develop a phase retrieval methodology to retrieve the out-of-plane component of magnetization. Based on our theory, we discuss suitable experimental conditions that would enable this imaging capability for magnetic materials and further extend to non-magnetic chiral materials.

47 OTHER INSTRUMENTATION↗

DOE OSTI2023

High‐Throughput Screening Assisted Discovery of a Stable Layered Anti‐Ferromagnetic Semiconductor: CdFeP 2 Se 6

Recent advances in 2D magnetism have heightened interest in layered magnetic materials due to their potential for spintronics. In particular, layered semiconducting antiferromagnets exhibit intriguing low-dimensional semiconducting behavior with both charge and spin as carrier controls. However, synthesis of these compounds is challenging and remains rare. Here, first-principles based high-throughput search is conducted to screen potentially stable mixed metal phosphorous trichalcogenides (MM ' P 2 X 6 , where M and M ' are transition metals and X is a chalcogenide) that have a wide range of tunable bandgaps and interesting magnetic properties. Among the potential candidates, a stable semiconducting layered magnetic material, CdFeP 2 Se 6 , that exhibits a short-range antiferromagnetic order at T N = 21 K with an indirect bandgap of 2.23 eV is successfully synthesized . This work suggests that high-throughput screening assisted synthesis can be an effective method for layered magnetic materials discovery.

2D materials↗

DOE OSTI2023

Electrical, optical, and magnetic properties of amorphous yttrium iron oxide thin films and consequences for non-local resistance measurements

We present magnetic characterization, charge resistivity, and optical photoluminescence measurements on amorphous yttrium iron oxide thin films ( ⁠a-Y–Fe–O), with supporting comparisons to amorphous germanium (⁠ a-Ge) films. We measured magnetic properties with both SQUID magnetometry and polarized neutron reflectometry. These results not only confirm that a-Y–Fe–O is a disordered magnetic material with strong predominantly antiferromagnetic exchange interactions and a high degree of frustration, but also that it is best understood electrically as a disordered semiconductor. As with amorphous germanium, a-Y–Fe–O obeys expectations for variable-range hopping through localized electron states over a wide range of temperature. We also clarify the consequences of charge transport through such a semiconducting medium for non-local voltage measurements intended to probe spin transport in nominally insulating magnetic materials. We further compare non-local resistance measurements made with “quasi-dc” automated current reversal to ac measurements made with a lock-in amplifier. These show that the “quasi-dc” measurement has an effective ac current excitation with frequency up to approximately 22 Hz, and that this effective ac excitation can cause artifacts in these measurements including incorrect sign of the non-local resistance. Here, this comprehensive investigation of non-local resistance measurements in a-Y–Fe–O shows no evidence of spin transport on micrometer length scales, which is contrary to our original work, and in line with more recent investigations by other groups.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2012

Influence of intergranular exchange coupling on the magnetization dynamics of CoCrPt:SiO{sub 2} granular media

We investigate the effect of Co{sup +} irradiation on the magnetization dynamics of CoCrPt:SiO{sub 2} granular media. Increasing irradiation levels reduce the saturation magnetization and effective anisotropy, which decrease the intrinsic magnetization precession frequency. Furthermore, increasing intergranular exchange coupling results in a qualitative change in the behavior of the magnetic material from a collection of individual grains to a homogeneous thin film, as evidenced in both the switching behavior and dynamics. The frequency change cannot be explained by single crystal macrospin modeling, and can only be reproduced by the inclusion of the dipolar effects and anisotropy distribution inherent in a granular medium.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2014

(Ca,Na)(Zn,Mn){sub 2}As{sub 2}: A new spin and charge doping decoupled diluted ferromagnetic semiconductor

Here, we report the successful synthesis of a spin- and charge-decoupled diluted magnetic semiconductor (DMS) (Ca,Na)(Zn,Mn){sub 2}As{sub 2}, crystallizing into the hexagonal CaAl{sub 2}Si{sub 2} structure. The compound shows a ferromagnetic transition with a Curie temperature up to 33 K with 10% Na doping, which gives rise to carrier density of n{sub p} ∼ 10{sup 20 }cm{sup −3}. The new DMS is a soft magnetic material with H{sub C} < 400 Oe. The anomalous Hall effect is observed below the ferromagnetic ordering temperature. With increasing Mn doping, ferromagnetic order is accompanied by an interaction between the local spin and mobile charge, giving rise to a minimum in resistivity at low temperatures and localizing the conduction electrons. The system provides an ideal platform for studying the interaction of the local spins and conduction electrons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

ALICE—An advanced reflectometer for static and dynamic experiments in magnetism at synchrotron radiation facilities

We report on significant developments of a high vacuum reflectometer (diffractometer) and spectrometer for soft x-ray synchrotron experiments which allows conducting a wide range of static and dynamic experiments. Although the chamber named ALICE was designed for the analysis of magnetic hetero- and nanostructures via resonant magnetic x-ray scattering, the instrument is not limited to this technique. The versatility of the instrument was testified by a series of pilot experiments. Static measurements involve the possibility to use scattering and spectroscopy synchrotron based techniques (photon-in photon-out, photon-in electron-out, and coherent scattering). Dynamic experiments require either laser or magnetic field pulses to excite the spin system followed by x-ray probe in the time domain from nano- to femtosecond delay times. In this temporal range, the demagnetization/remagnetization dynamics and magnetization precession in a number of magnetic materials (metals, alloys, and magnetic multilayers) can be probed in an element specific manner. We demonstrate here the capabilities of the system to host a variety of experiments, featuring ALICE as one of the most versatile and demanded instruments at the Helmholtz Center in Berlin-BESSY II synchrotron center in Berlin, Germany.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2018

Superexchange Interaction in Magnetic Insulators with Spin Crossover

We present the derivation of a microscopic superexchange Hamiltonian for undoped magnetic insulators with an arbitrary spin. It is established that the sign of the (ferromagnetic or antiferromagnetic) superexchange between magnetic ions in the d{sup n} configuration depends on the spin nature of virtual multielectron states d{sup n± 1}, viz., low-spin or high-spin partners with S ± 1/2 relative to ground state of the d{sup n} configuration with spin S. A macroscopic substantiation is given for the Goodenough–Kanamori rules and simple mean-field estimates connecting the magnetic ordering temperature with the exchange constant. The conventional Anderson superexchange for magnetic materials with spin S = 1/2 and the P/T magnetic phase diagram for ferroborate FeBO{sub 3} with spin crossover S = (5/2 ↔ 1/2) at the Fe{sup 3+} ion under a high pressure are also reproduced as a test.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1960

The U. S. Space Program -- An Appraisal

The National Aeronautics and Space Administration has a significant interest in research on magnetic materials and in developing a better understanding of magnetic phenomena here on earth, in space and in the vicinity of the other planets of our solar system. But it would be presumptuous of me, an ordinary administrator, to lecture to this distinguished group of experts in the field on the subject of magnetism and magnetic materials. Instead, I propose to tell you briefly about the dimensions and principal areas of effort of the program we are pursuing in space research. Naturally, I will identify the nature of our interest in the specialty with which you are concerned. Finally, I want to attempt an assessment of the United States program in space exploration with perhaps a sidelong glance at the comparable efforts of our principal competitor in this field -- the Soviet Union. In the preparation of this paper, I have had the assistance of several very able scientists who are members of our staff at NASA.

Glennan, T. Keith↗

DOE OSTI2014

Stimuli-responsive hybrid materials: breathing in magnetic layered double hydroxides induced by a thermoresponsive molecule

In this study, a hybrid magnetic multilayer material of micrometric size, with highly crystalline hexagonal crystals consisting of CoAl–LDH ferromagnetic layers intercalated with thermoresponsive 4-(4 anilinophenylazo)benzenesulfonate (AO5) molecules diluted (ratio 9 : 1) with a flexible sodium dodecylsulphate (SDS) surfactant has been obtained. The resulting material exhibits thermochromism attributable to the isomerization between the azo (prevalent at room temperature) and the hydrazone (favoured at higher temperatures) tautomers, leading to a thermomechanical response. In fact, these crystals exhibited thermally induced motion triggering remarkable changes in the crystal morphology and volume. In situ variable temperature XRD of these thin hybrids shows that the reversible change into the two tautomers is reflected in a shift of the position of the diffraction peaks at high temperatures towards lower interlayer spacing for the hydrazone form, as well as a broadening of the peaks reflecting lower crystallinity and ordering due to non-uniform spacing between the layers. These structural variations between room temperature (basal spacing (BS) = 25.91 Å) and 100 °C (BS = 25.05 Å) are also reflected in the magnetic properties of the layered double hydroxide (LDH) due to the variation of the magnetic coupling between the layers. Finally and in conclusion, our study constitutes one of the few examples showing fully reversible thermo-responsive breathing in a 2D hybrid material. In addition, the magnetic response of the hybrid can be modulated due to the thermotropism of the organic component that, by influencing the distance and in-plane correlation of the inorganic LDH, modulates the magnetism of the CoAl–LDH sheets in a certain range.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Demagnetization analysis of an 18 GHz electron cyclotron resonance ion source permanent magnet hexapole

An upgrade of ECR2 at the Argonne Tandem Linac Accelerator System is under way, focusing on increasing the intensity capabilities of the facility. ECR2 is a room temperature electron cyclotron resonance ion source, and the upgrade has strict requirements to retain radial access to the plasma chamber and keep the ion source operating without the use of superconducting magnets. The upgrade design with respect to the magnet arrangement and magnetization vectors has recently been presented [R. C. Vondrasek, J. McLain, and R. H. Scott, J. Phys.: Conf. Ser. 2743 , 012044 (2024)] using the same magnetic material as the current ECR2 hexapole. A thorough exploration of the demagnetization potential of this hexapole was carried out, and the risk of demagnetization was deemed too high, despite the magnetic performance meeting the requirements for the upgrade. Additional permanent magnet materials are considered with their respective performance evaluated. Magnet strength and demagnetization resistance are investigated and optimized with the final room temperature design demonstrating a high temperature transient demagnetization resistance and a radial magnetic field of 1.18 T at the plasma chamber wall. Finally, the simulations of this hexapole suggest that it will be sufficient to optimize intensity with a 14.5 GHz driving frequency and will allow 18 GHz operation, while keeping a high safety margin for maintaining magnet performance.

Argonne Tandem Linac Accelerator System↗

DOE OSTI2014

Spin-phonon coupling in BaFe{sub 12}O{sub 19} M-type hexaferrite

The spin-phonon coupling in magnetic materials is due to the modulation of the exchange integral by lattice vibrations. BaFe{sub 12}O{sub 19} M-type hexaferrite, which is the most used magnetic material as permanent magnet, transforms into ferrimagnet at high temperatures, but no spin-phonon coupling was previously observed at this transition. In this letter, we investigated the temperature-dependent Raman spectra of polycrystalline BaFe{sub 12}O{sub 19} M-type hexaferrite from room temperature up to 780 K to probe spin-phonon coupling at the ferrimagnetic transition. An anomaly was observed in the position of the phonon attributed to the Fe{sup (4)}O{sub 6}, Fe{sup (5)}O{sub 6}, and Fe{sup (1)}O{sub 6} octahedra, evidencing the presence of a spin-phonon coupling in BaM in the ferrimagnetic transition at 720 K. The results also confirmed the spin-phonon coupling is different for each phonon even when they couple with the same spin configuration.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1981

Hard permanent magnet development trends and their application to A.C. machines

The physical and magnetic properties of Mn-Al-C, Fe-Cr-Co, and RE-TM (rare earth-transition metal intermetallics) in polymer and soft metal bonded or sintered form are considered for ac circuit machine usage. The manufacturing processes for the magnetic materials are reviewed, and the mechanical and electrical properties of the magnetic materials are compared, with consideration given to the reference Alnico magnet. The Mn-Al-C magnets have the same magnetic properties and costs as Alnico units, operate well at low temperatures, but have poor high temperature performance. Fe-Cr-Co magnets also have comparable cost to Alnico magnets, and operate at high or low temperature, but are brittle, expensive, and contain Co. RE-Co magnets possess a high energy density, operate well in a wide temperature range, and are expensive. Recommendation for exploring the rare-earth alternatives are offered.

Mildrum, H. F.↗

DOE OSTI2021

Exploring a quantum-information-relevant magnonic material: Ultralow damping at low temperature in the organic ferrimagnet V[TCNE]x

Quantum information science and engineering require novel low-loss magnetic materials for magnon-based quantum-coherent operations. The search for low-loss magnetic materials, traditionally driven by applications in microwave electronics near room temperature, has gained additional constraints from the need to operate at cryogenic temperatures for many applications in quantum information science and technology. Whereas yttrium iron garnet (YIG) has been the material of choice for decades, the emergence of molecule-based materials with robust magnetism and ultra-low damping has opened new avenues for exploration. Specifically, thin films of vanadium tetracyanoethylene (V[TCNE]x) can be patterned into the multiple, connected structures needed for hybrid quantum elements and have shown room-temperature Gilbert damping (α = 4 × 10−5) that rivals the intrinsic (bulk) damping otherwise seen only in highly polished YIG spheres (far more challenging to integrate into arrays). Here, the authors present a comprehensive and systematic study of the low-temperature magnetization dynamics for V[TCNE]x thin films, with implications for their application in quantum systems. These studies reveal a temperature-driven, strain-dependent magnetic anisotropy that compensates the thin-film shape anisotropy and the recovery of a magnetic resonance linewidth at 5 K that is comparable to room-temperature values (roughly 2 G at 9.4 GHz). The authors can account for these variations of the V[TCNE]x linewidth within the context of scattering from very dilute paramagnetic impurities and anticipate additional linewidth narrowing as the temperature is further reduced.

Yusuf, H. (ORCID:0000000194627928)↗

NASA NTRS1980

Electric vehicle traction motors - The development of an advanced motor concept

An axial-field permanent magnet traction motor is described, similar to several advanced motors that are being developed in the United States. This type of machine has several advantages over conventional dc motors, particularly in the electric vehicle application. The rapidly changing cost of magnetic materials, particularly cobalt, makes it important to study the utilization of permanent magnet materials in such machines. The impact of different magnets on machine design is evaluated, and the advantages of using iron powder composites in the armature are assessed.

Campbell, P.↗

DOE OSTI2013

Artificial Spin Ice: Controlling Geometry, Engineering Frustration

Frustration – the presence of competing interactions – is ubiquitous in the physical sciences and is a source of degeneracy and disorder, which in turn give rise to new and interesting physical phenomena. Perhaps nowhere does it occur more simply than in correlated spin systems, where it has been studied in the most detail. In disordered magnetic materials, frustration leads to spin-glass phenomena, with analogies to the behavior of structural glasses and neural networks. In structurally ordered magnetic materials, it has also been the topic of extensive theoretical and experimental studies over the past two decades. Such geometrical frustration has opened a window on a wide range of fundamentally new exotic behavior. This includes spin liquids in which the spins continue to fluctuate down to the lowest temperatures; and spin ice, which appears to retain macroscopic entropy even in the low temperature limit where it enters a topological Coulomb phase. In the past seven years a new perspective has opened in the study of frustration through the creation of artificial frustrated magnetic systems. These materials consist of arrays of lithographically fabricated single-domain ferromagnetic nanostructures that behave like giant Ising spins. The nanostructures’ interactions can be controlled through appropriate choices of their geometric properties and arrangement on a (frustrated) lattice. The degrees of freedom of the material can not only be directly tuned, but also individually observed. Experimental studies have unearthed intriguing connections to the out-of-equilibrium physics of disordered systems and non-thermal ‘granular’ materials, while revealing strong analogies to (spin) ice materials and their fractionalized magnetic monopole excitations, lending the enterprise a distinctly interdisciplinary flavor. The experimental results have also been closely coupled to theoretical and computational analyses, facilitated by connections to classic models of frustrated magnetism, whose hitherto unobserved aspects have here found an experimental realization. We review the considerable experimental and theoretical progress in this field, including connections to other frustrated phenomena, and we outline future vistas for progress in this rapidly expanding field.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Electrical Interrogation of Thickness‐Dependent Multiferroic Phase Transitions in the 2D Antiferromagnetic Semiconductor NiI 2

Abstract 2D magnetic materials hold promise for quantum and spintronic applications. 2D antiferromagnetic materials are of particular interest due to their relative insensitivity to external magnetic fields and higher switching speeds compared to 2D ferromagnets. However, their lack of macroscopic magnetization impedes detection and control of antiferromagnetic order, thus motivating magneto‐electrical measurements for these purposes. Additionally, many 2D magnetic materials are ambient‐reactive and electrically insulating or highly resistive below their magnetic ordering temperatures, which imposes severe constraints on electronic device fabrication and characterization. Herein, these issues are overcome via a fabrication protocol that achieves electrically conductive devices from the ambient‐reactive 2D antiferromagnetic semiconductor NiI 2 . The resulting gate‐tunable transistors show band‐like electronic transport below the antiferromagnetic and multiferroic transition temperatures of NiI 2 , revealing a Hall mobility of 15 cm 2 V −1 s −1 at 1.7 K. These devices also allow direct electrical probing of the thickness‐dependent multiferroic phase transition temperature of NiI 2 from 59 K (bulk) to 28 K (monolayer).

2D magnets↗

DOE OSTI2011

What Can we Learn About Battery Materials from Their Magnetic Properties

Electrode materials for Li-ion batteries should combine electronic and ionic conductivity, structural integrity, and safe operation over thousands of lithium insertion and removal cycles. The quest for higher energy density calls for better understanding of the redox processes, charge and mass transfer occurring upon battery operation. A number of techniques have been used to characterize long-range and local structure, electronic and ionic transport in bulk of active materials and at interfaces, with an ongoing move toward in situ techniques determining the changes as they happen. This paper reviews several representative examples of using magnetic properties toward understanding of Li-ion battery materials with a notion to highlight the intimate connection between the magnetism, electronic and atomic structure of solids, and to demonstrate how this connection has been used to reveal the fine electronic and atomic details related to the electrochemical performance of the battery materials.

36 MATERIALS SCIENCE↗

NASA NTRS2018

Magnetic Properties of Fe-49Co-2V Alloy and Pure Fe at Room and Elevated Temperatures

The National Aeronautics and Space Administration (NASA) has a need for soft magnetic materials for fission power and ion propulsion systems. In this work the magnetic properties of the soft magnetic materials Hiperco 50 (Fe-49wt%Cr-2V) and CMI-C (commercially pure magnetic iron) were examined at various temperatures up to 600 C. Toroidal Hiperco 50 samples were made from stacks of 0.35 mm thick sheet, toroidal CMI-C specimens were machined out of solid bar stock, and both were heat treated prior to testing. The magnetic properties of a Hiperco 50 sample were measured at various temperatures up to 600 C and then again after returning to room temperature; the magnetic properties of CMI-C were tested at temperatures up to 400 C. For Hiperco 50 coercivity decreased as temperature increased, and remained low upon returning to room temperature; maximum permeability improved (increased) with increasing temperature and was dramatically improved upon returning to room temperature; remanence was not significantly affected by temperature; flux density at H = 0.1 kA/m increased slightly with increasing temperature, and was about 20% higher upon returning to room temperature; flux density at H = 0.5 kA/m was insensitive to temperature. It appears that the properties of Hiperco 50 improved with increasing temperature due to grain growth. There was no significant magnetic property difference between annealed and aged CMI-C iron material; permeability tended to decrease with increasing temperature; the approximate decline in the permeability at 400 C compared to room temperature was 30%; saturation flux density, B(sub S), was approximately equal for all temperatures below 400 C; B(sub S) was lower at 400 C.

De Groh, Henry C., III↗