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DOE OSTI2018

Unraveling Nanoscale Magnetic Ordering in Fe3O4 Nanoparticle Assemblies via X-rays

Understanding the correlations between magnetic nanoparticles is important for nanotechnologies, such as high-density magnetic recording and biomedical applications, where functionalized magnetic particles are used as contrast agents and for drug delivery. The ability to control the magnetic state of individual particles depends on the good knowledge of the magnetic correlations between particles when assembled. Inaccessible via standard magnetometry techniques, nanoscale magnetic ordering in self-assemblies of Fe3O4 nanoparticles is here unveiled via X-ray resonant magnetic scattering (XRMS). Measured throughout the magnetization process, the XRMS signal reveals size-dependent inter-particle magnetic correlations. Smaller (5 nm) particles show little magnetic correlations, even when packed close together, yielding to magnetic disorder in the absence of an external field, i.e., superparamagnetism. In contrast, larger (11 nm) particles tend to be more strongly correlated, yielding a mix of magnetic orders including ferromagnetic and anti-ferromagnetic orders. These magnetic correlations are present even when the particles are sparsely distributed.

Chesnel, Karine↗

DOE OSTI2019

Investigation of Powder Processing, Heat Treating, and Texturing to Improve Gas Atomized alnico Magnets for use in Electric Drive Motors

Alnico permanent magnet materials have been proposed as a rare earth free permanent magnet alternative during an ongoing search to replace rare earth permanent magnets that are used for interior permanent magnet motors, a common motor found in electric vehicles. A powder processing approach was used to study two alnico alloys (Full-Co and lower cost Co-Lean, both with enhanced coercivity) to anticipate high volume manufacturing needed to supply millions of permanent magnets to interior permanent magnet motors. In this study the two alloys were gas atomized, compression molded, and solid-state sintered to fabricate near-final shape alnico magnets. The Full-Co displayed abnormal grain growth (resulting in >1 mm size grains) during sintering while the Co-Lean did not (~20 μm – 400 μm sized grains depending on the sintering hold times). Solid state grain alignment was used to promote a <001> textured (easy axis) microstructure to enhance magnetic properties, yet both alloys did not show predicted grain alignment behavior. Comparisons of the powder processing, microstructures, and magnetic properties of the two alloys will be discussed, as well as an evaluation as to why non-theoretical processing behavior of the Full-Co and Co-Lean alnico permanent magnets is occurring. Preliminary interior permanent magnet motor designs for alnico magnets are discussed, as this is the overarching objective for powder-based alnico permanent magnets.

Rinko, Emily↗

DOE OSTI2024

ASb 3 Mn 9 O 19 (A = K or Rb): New Mn-Based 2D Magnetoplumbites with Geometric and Magnetic Frustration

Magnetoplumbites are one of the most broadly studied families of hexagonal ferrites, typically with high magnetic ordering temperatures, making them excellent candidates for permanent magnets. However, magnetic frustration is rarely observed in magnetoplumbites. Herein, the discovery, synthesis, and characterization of the first Mn-based magnetoplumbite, as well as the first magnetoplumbite involving pnictogens (Sb), ASb 3 Mn 9 O 19 (A = K or Rb) are reported. The Mn 3+ ( S = 2) cations, further confirmed by DC magnetic susceptibility and X-ray photoelectron spectroscopy, construct three geometrically frustrated sublattices, including Kagome, triangular, and puckered honeycomb lattices. Magnetic properties measurements revealed strong antiferromagnetic spin–spin coupling as well as multiple low-temperature magnetic features. Heat capacity data does not show any prominent λ-anomaly, suggesting minimal associated magnetic entropy. Moreover, neutron powder diffraction (NPD) implied the absence of long-range magnetic ordering in KSb 3 Mn 9 O 19 down to 3 K. However, several magnetic peaks are observed in RbSb 3 Mn 9 O 19 at 3 K, corresponding to an incommensurate magnetic structure. Interestingly, strong diffuse scattering is seen in the NPD patterns of both compounds at low angles and is analyzed by reverse Monte Carlo refinements, indicating short-range spin ordering related to frustrated magnetism as well as 2D magnetic correlations in ASb 3 Mn 9 O 19 (A = K or Rb).

2-D magnetic correlation↗

DOE OSTI2014

Magnetic and magnetocaloric properties of La{sub 0.6}Pr{sub 0.1}Sr{sub 0.3}Mn{sub 1−x}Fe{sub x}O{sub 3} (0≤x≤0.3) manganites

The La{sub 0.6}Pr{sub 0.1}Sr{sub 0.3}Mn{sub 1−x}Fe{sub x}O{sub 3} (x=0, 0.1, 0.2 and 0.3) samples have been elaborated by the solid-state reaction method. X-ray powder diffraction shows that all the samples crystallize in a rhombohedric phase with R3{sup ¯}c space group. The variation of magnetization as a function of temperature and applied magnetic field was carried out. The samples for x=0 and 0.1 exhibit a FM–PM transition at the Curie temperature T{sub C}, however, for x=0.2 and 0.3 exhibit an AFM–PM one at the Neel temperature T{sub N}, when the temperature increases. A magneto-caloric effect has been calculated in terms of isothermal magnetic entropy change. A large magneto-caloric effect has been observed, the maximum entropy change, |ΔS{sub M}{sup max}|, reaches the highest value of 3.28 J/kgK under a magnetic field change of 5 T with an RCP value of 220 J/kg for La{sub 0.6}Pr{sub 0.1}Sr{sub 0.3}MnO{sub 3} composition, which will be an interesting compound for application materials working as magnetic refrigerants near room temperature. - Graphical abstract: Magnetic entropy change versus temperature and applied magnetic field for x=0.1 (a) and RCP versus applied magnetic field for x=0, 0.1 (b). - Highlights: • The La{sub 0.6}Pr{sub 0.1}Sr{sub 0.3}Mn{sub 1−x}Fe{sub x}O{sub 3} (0≤x≤0.3) polycrystalline samples were prepared by the solid state reaction method. • Crystalline and magnetic structures were investigated using DRX and magnetization measurements. • The magnetocaloric (MC) effect was estimated versus magnetic field and temperatures. • Compounds with x=0, 0.1 exhibit great potential for magnetic refrigeration at room temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Tri-axial magnetic anisotropies in RE{sub 2}Ba{sub 4}Cu{sub 7}O{sub 15−y} superconductors

We report a novel quantification method of tri-axial magnetic anisotropy in orthorhombic substances containing rare earth (RE) ions using tri-axial magnetic alignment and tri-axial magnetic anisotropies depending on the type of RE in RE-based cuprate superconductors. From the changes in the axes for magnetization in magnetically aligned powders of (RE′{sub 1−x}RE″{sub x}){sub 2}Ba{sub 4}Cu{sub 7}O{sub y} [(RE′,RE″)247] containing RE ions with different single-ion magnetic anisotropies, the ratios of three-dimensional magnetic anisotropies between RE′247 and RE″247 could be determined. The results in (Y,Er)247, (Dy,Er)247, (Ho,Er)247, and (Y,Eu)247 systems suggest that magnetic anisotropies largely depended on the type of RE′ (or RE″), even in the heavy RE ions with higher magnetic anisotropies. An appropriate choice of RE ions in RE-based cuprate superconductors enables the reduction of the required magnetic field for the production of their bulks and thick films based on the tri-axial magnetic alignment technique using modulated rotation magnetic fields.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2016

A general nonlinear magnetomechanical model for ferromagnetic materials under a constant weak magnetic field

Weak magnetic nondestructive testing (e.g., metal magnetic memory method) concerns the magnetization variation of ferromagnetic materials due to its applied load and a weak magnetic surrounding them. One key issue on these nondestructive technologies is the magnetomechanical effect for quantitative evaluation of magnetization state from stress–strain condition. A representative phenomenological model has been proposed to explain the magnetomechanical effect by Jiles in 1995. However, the Jiles' model has some deficiencies in quantification, for instance, there is a visible difference between theoretical prediction and experimental measurements on stress–magnetization curve, especially in the compression case. Based on the thermodynamic relations and the approach law of irreversible magnetization, a nonlinear coupled model is proposed to improve the quantitative evaluation of the magnetomechanical effect. Excellent agreement has been achieved between the predictions from the present model and previous experimental results. In comparison with Jiles' model, the prediction accuracy is improved greatly by the present model, particularly for the compression case. A detailed study has also been performed to reveal the effects of initial magnetization status, cyclic loading, and demagnetization factor on the magnetomechanical effect. Our theoretical model reveals that the stable weak magnetic signals of nondestructive testing after multiple cyclic loads are attributed to the first few cycles eliminating most of the irreversible magnetization. Remarkably, the existence of demagnetization field can weaken magnetomechanical effect, therefore, significantly reduces the testing capability. This theoretical model can be adopted to quantitatively analyze magnetic memory signals, and then can be applied in weak magnetic nondestructive testing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2014

THE IMPORTANCE OF THE MAGNETIC FIELD FROM AN SMA-CSO-COMBINED SAMPLE OF STAR-FORMING REGIONS

Submillimeter dust polarization measurements of a sample of 50 star-forming regions, observed with the Submillimeter Array (SMA) and the Caltech Submillimeter Observatory (CSO) covering parsec-scale clouds to milliparsec-scale cores, are analyzed in order to quantify the magnetic field importance. The magnetic field misalignment δ—the local angle between magnetic field and dust emission gradient—is found to be a prime observable, revealing distinct distributions for sources where the magnetic field is preferentially aligned with or perpendicular to the source minor axis. Source-averaged misalignment angles (|δ|) fall into systematically different ranges, reflecting the different source-magnetic field configurations. Possible bimodal (|δ|) distributions are found for the separate SMA and CSO samples. Combining both samples broadens the distribution with a wide maximum peak at small (|δ|) values. Assuming the 50 sources to be representative, the prevailing source-magnetic field configuration is one that statistically prefers small magnetic field misalignments |δ|. When interpreting |δ| together with a magnetohydrodynamics force equation, as developed in the framework of the polarization-intensity gradient method, a sample-based log-linear scaling fits the magnetic field tension-to-gravity force ratio (Σ {sub B}) versus (|δ|) with (Σ {sub B}) = 0.116 · exp (0.047 · (|δ|)) ± 0.20 (mean error), providing a way to estimate the relative importance of the magnetic field, only based on measurable field misalignments |δ|. The force ratio Σ {sub B} discriminates systems that are collapsible on average ((Σ {sub B}) < 1) from other molecular clouds where the magnetic field still provides enough resistance against gravitational collapse ((Σ {sub B}) > 1). The sample-wide trend shows a transition around (|δ|) ≈ 45°. Defining an effective gravitational force ∼1 – (Σ {sub B}), the average magnetic-field-reduced star formation efficiency is at least a factor of two smaller than the free-fall efficiency. For about one fourth of the sources the average efficiency drops to zero. The force ratio Σ {sub B} can further be linked to the normalized mass-to-flux ratio, yielding an estimate for the latter one without the need of field strength measurements. Across the sample, a transition from magnetically supercritical to subcritcal is observed with growing misalignment (|δ|)

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2018

Model-Based Iterative Reconstruction of Magnetization Using Vector Field Electron Tomography

Vector field electron tomography (VFET) is extensively used for three-dimensional (3-D) imaging of magnetic materials at nanometer resolutions. The conventional approach is to reconstruct and visualize the magnetic vector potential or the magnetic field associated with the sample. There is a lack of algorithms capable of reconstructing the 3-D distribution of magnetization from VFET data. Unlike magnetic vector potential and magnetic field, magnetization is a fundamental physical property of the sample that does not extend beyond the dimensions of the sample. We present a model-based iterative reconstruction algorithm (MBIR) that reconstructs the magnetization by minimizing a cost function consisting of a forward model term and a prior model term. The forward model uses the physics of imaging to model the VFET data as a function of the magnetization, and the prior model enforces sparsity in the magnetization reconstruction. We then formulate an optimization algorithm based on the theory of alternate direction method of multipliers to minimize the resulting MBIR cost function. In conclusion, using simulated and real data, we show that our algorithm accurately reconstructs both the magnetization and the magnetic vector potential.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2014

WE-G-17A-09: Novel Magnetic Shielding Design for Inline and Perpendicular Integrated 6 MV Linac and 1.0 T MRI Systems

Purpose: The influence of fringe magnetic fields delivered by magnetic resonance imaging (MRI) on the beam generation and transportation in Linac is still a major challenge for the integration of linear accelerator and MRI (Linac-MRI). In this study, we investigated an optimal magnetic shielding design for Linac-MRI and further characterized the beam trajectory in electron gun. Methods: Both inline and perpendicular configurations were analyzed in this study. The configurations, comprising a Linac-MRI with a 100cm SAD and an open 1.0 T superconductive magnet, were simulated by the 3D finite element method (FEM). The steel shielding around the Linac was included in the 3D model, the thickness of which was varied from 1mm to 20mm, and magnetic field maps were acquired with and without additional shielding. The treatment beam trajectory in electron gun was evaluated using OPERA 3d SCALA with and without shielding cases. Results: When Linac was not shielded, the uniformity of diameter sphere volume (DSV) (30cm) was about 5 parts per million (ppm) and the fringe magnetic fields in electron gun were more than 0.3 T. With shielding, the magnetic fields in electron gun were reduced to less than 0.01 T. For the inline configuration, the radial magnetic fields in the Linac were about 0.02T. A cylinder steel shield used (5mm thick) altered the uniformity of DSV to 1000 ppm. For the perpendicular configuration, the Linac transverse magnetic fields were more than 0.3T, which altered the beam trajectory significantly. A 8mm-thick cylinder steel shield surrounding the Linac was used to compensate the output losses of Linac, which shifted the magnetic fields' uniformity of DSV to 400 ppm. Conclusion: For both configurations, the Linac shielding was used to ensure normal operation of the Linac. The effect of magnetic fields on the uniformity of DSV could be modulated by the shimming technique of the MRI magnet. NIH/NIGMS grant U54 GM104944, Lincy Endowed Assistant Professorship.

43 PARTICLE ACCELERATORS↗

DOE OSTI2015

Technical Note: Response measurement for select radiation detectors in magnetic fields

Purpose: Dose response to applied magnetic fields for ion chambers and solid state detectors has been investigated previously for the anticipated use in linear accelerator–magnetic resonance devices. In this investigation, the authors present the measured response of selected radiation detectors when the magnetic field is applied in the same direction as the radiation beam, i.e., a longitudinal magnetic field, to verify previous simulation only data. Methods: The dose response of a PR06C ion chamber, PTW60003 diamond detector, and IBA PFD diode detector is measured in a longitudinal magnetic field. The detectors are irradiated with buildup caps and their long axes either parallel or perpendicular to the incident photon beam. In each case, the magnetic field dose response is reported as the ratio of detector signals with to that without an applied longitudinal magnetic field. The magnetic field dose response for each unique orientation as a function of magnetic field strength was then compared to the previous simulation only studies. Results: The measured dose response of each detector in longitudinal magnetic fields shows no discernable response up to near 0.21 T. This result was expected and matches the previously published simulation only results, showing no appreciable dose response with magnetic field. Conclusions: Low field longitudinal magnetic fields have been shown to have little or no effect on the dose response of the detectors investigated and further lend credibility to previous simulation only studies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2022

Competing Easy-Axis Anisotropies Impacting Magnetic Tunnel Junction-Based Molecular Spintronics Devices (MTJMSDs)

Molecular spintronics devices (MSDs) attempt to harness molecules’ quantum state, size, and configurable attributes for application in computer devices—a quest that began more than 70 years ago. In the vast number of theoretical studies and limited experimental attempts, MSDs have been found to be suitable for application in memory devices and futuristic quantum computers. MSDs have recently also exhibited intriguing spin photovoltaic-like phenomena, signaling their potential application in cost-effective and novel solar cell technologies. The molecular spintronics field’s major challenge is the lack of mass-fabrication methods producing robust magnetic molecule connections with magnetic electrodes of different anisotropies. Another main challenge is the limitations of conventional theoretical methods for understanding experimental results and designing new devices. Magnetic tunnel junction-based molecular spintronics devices (MTJMSDs) are designed by covalently connecting paramagnetic molecules across an insulating tunneling barrier. The insulating tunneling barrier serves as a mechanical spacer between two ferromagnetic (FM) electrodes of tailorable magnetic anisotropies to allow molecules to undergo many intriguing phenomena. Our experimental studies showed that the paramagnetic molecules could produce strong antiferromagnetic coupling between two FM electrodes, leading to a dramatic large-scale impact on the magnetic electrode itself. Recently, we showed that the Monte Carlo Simulation (MCS) was effective in providing plausible insights into the observation of unusual magnetic domains based on the role of single easy-axis magnetic anisotropy. Here, we experimentally show that the response of a paramagnetic molecule is dramatically different when connected to FM electrodes of different easy-axis anisotropies. Motivated by our experimental studies, here, we report on an MCS study investigating the impact of the simultaneous presence of two easy-axis anisotropies on MTJMSD equilibrium properties. In-plane easy-axis anisotropy produced multiple magnetic phases of opposite spins. The multiple magnetic phases vanished at higher thermal energy, but the MTJMSD still maintained a higher magnetic moment because of anisotropy. The out-of-plane easy-axis anisotropy caused a dominant magnetic phase in the FM electrode rather than multiple magnetic phases. The simultaneous application of equal-magnitude in-plane and out-of-plane easy-axis anisotropies on the same electrode negated the anisotropy effect. Our experimental and MCS study provides insights for designing and understanding new spintronics-based devices.

42 ENGINEERING↗

DOE OSTI2024

Recycling of additively printed anisotropic Nd-Fe-B bonded magnets

A high potential cost-effective and environmentally friendly method has been applied for recycling anisotropic Nd-Fe-B bonded magnets. Waste additively printed Hydrogenation-Disproportionation-Desorption-Recombination (HDDR) Nd-Fe-B anisotropic bonded magnet was pulverized into composite powder containing Nd-Fe-B particles and nylon binder through cryomilling at a liquid nitrogen temperature (~77 K) under Ar inert atmosphere. Then, the cryomilled composite powder was warm compacted into a bonded magnet. Further, the magnetic particles were aligned during post-compaction annealing under a magnetic field of 30 kOe. The recycled bonded magnets have a higher density (3% enhancement), but slightly inferior magnetic properties compared to the original magnets, i.e., the magnetic remanence, coercivity and maximum energy product are reduced by 2%, 3% and 8%, respectively. The scanning electron microscopy revealed that some HDDR Nd-Fe-B powder crumbled into fine particles during cryomilling. Powder X-ray diffraction showed a small amount of Nd-oxide impurity in the cryomilled powder. The slightly deteriorated magnetic properties are ascribed to the oxidation of Nd-Fe-B particles due to formation of fresh fracture surface during cryomilling. The approach enables the direct reuse of end-of-life bonded magnets in an economical and environmentally friendly way.

36 MATERIALS SCIENCE↗

DOE OSTI2024

High-order harmonics and the reverse of the squaring up process in the triangular-lattice magnet HoPdAl 4 ⁢Ge 2

We uncover high-order harmonics and the reverse of the squaring-up process, in terms of analyzing the evolution of magnetic orders in a centrosymmetric layered triangular-lattice magnet HoPdAl 4 ⁢Ge 2 , based on a detailed study of the crystal structure, magnetic susceptibility, magnetization, heat capacity, and magnetic structure. Temperature dependencies of magnetic susceptibility and heat capacity show two magnetic transitions at T N = 10.5 K and T t = 5.5 K. Below T N , Ho 3+ spins order antiferromagnetically as a transverse spin-density wave with the propagation vector k 1 = (001.5 – δ) with δ ≈ 0.18. Upon further cooling through T t , the high-order harmonics with k n = (001.5 – nδ), n = 3, 5, 7 develop, suggesting a squaring-up process. It is surprising that the squaring-up process does not continue down to 0 K but reverses the trend below 3 K. Magnetic-field-induced metastable transitions were observed in M⁡(H) curves with the fields applied both parallel and perpendicular to the triangular-lattice plane. Neutron-diffraction results suggest that the magnetization process in HoPdAl 4 ⁢Ge 2 involves the conversion of k n = (001.5 – n⁢δ) with n = 1, 3, 5, 7, to a ferromagnetic k F = (000) component. It is worth noting that the already weak seventh harmonic magnetic peak is enhanced by applying a small magnetic field in the ab plane at 1.5 K or warming up to 3 K, accompanied by a slight decrease of δ.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2019

New Approach and Test Facility for High Field Accelerator Magnets R&D

This paper presents a new approach for developing and demonstrating high field magnet technology based on a magnet and test facility developed specifically for it. The traditional approach for carrying out high field magnet R&D has been building a new magnet to demonstrate a new design, new material or new technology. However, building a high field magnet is time consuming and expensive. To overcome this limitation, Brookhaven National Laboratory (BNL) built and successfully tested a 10 T Nb 3 Sn dipole DCC017 with large enough open or clear space (31 mm wide and 338 mm high) so that a pair of racetrack coils could be inserted into this opening without disassembling the magnet. The motivation be-hind this design was to facilitate a magnet R&D program where the new coils (with a large range in width and height accommodated) would reside in a high field region in direct contact with the existing coils (just as other magnet coils) and thus become an integral part of the magnet. We summarize the approach, the magnet, the test facility, past experiences, current and future test plans and planned up-grade. Here, the magnet facility is now available to service the needs of the wider community for testing cable and insert coils in a back-ground field of up to 10 T.

43 PARTICLE ACCELERATORS↗

DOE OSTI2016

Studies on in situ magnetic alignment of bonded anisotropic Nd-Fe-B alloy powders

We presented some considerations for achieving high degree of alignment in polymer bonded permanent magnets via the results of a study on in situ magnetic alignment of anisotropic Nd-Fe-B magnet powders. Contributions from effect of the alignment temperature, alignment magnetic field and the properties of the polymer on the hard magnetic properties of the bonded magnet were considered. Moreover, the thermo-rheological properties of the polymer and the response of the magnet powders to the applied magnetic field indicate that hard magnetic properties were optimized at an alignment temperature just above the melting temperature of the EVA co-polymer. This agrees with an observed correlation between the change in magnetization due to improved magnetic alignment of the anisotropic powders and the change in viscosity of the binder. Finally, manufacturing cost can be minimized by identifying optimum alignment temperatures and magnetic field strengths.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Deconvolution of X-ray natural and magnetic circular dichroism in chiral Dy-ferroborate

Structural chirality and magnetism, when intertwined, can have profound implications on materials properties. Using X-ray imaging and spectroscopic measurements that leverage the natural and magnetic circular dichroic effects present in magnetized chiral crystal structures, we probe the interplay between chirality and magnetism across the field-induced spin-flop transition of Dy ferroborate, DyFe 3 (BO 3 ) 4 . Deconvolution of natural and magnetic circular dichroic signals at the Fe K and Dy L 2,3 absorption edges of the non-centrosymmetric structure was enabled by use of tunable temperature and magnetic field, providing access to element-specific magnetic information across the spin-flop transition. The magnetic response of Fe and Dy sublattices was found to be independent of domain chirality. The chiral domains were robust against both the (chirality preserving) R32 to P3 1 21/P3 2 21 structural phase transition at 280 K, and application of magnetic field up to 4 Tesla. A third flavor of X-ray dichroism, magneto-chiral dichroism, was not detected within the accuracy of our measurements. The absence of significant Fe magnetization along the screw, c-axis for the magnetic field strength used in this study, together with non-linear coupling of magnetic field to electric polarization across the spin-flop transition, may hinder observation of magneto-chiral dichroic effects in this system.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2015

Size effects in the magnetic properties of ε-Fe{sub 2}O{sub 3} nanoparticles

We report the results of comparative analysis of magnetic properties of the systems based on ε-Fe{sub 2}O{sub 3}, nanoparticles with different average sizes (from ∼3 to 9 nm) and dispersions. The experimental data for nanoparticles higher than 6–8 nm in size are consistent with the available data, specifically, the transition to the magnetically ordered state occurs at a temperature of ∼500 K and the anomalies of magnetic properties observed in the range of 80–150 K correspond to the magnetic transition. At the same time, Mőssbauer and ferromagnetic resonance spectroscopy data as well as the results of static magnetic measurements show that at room temperature all the investigated samples contain ε-Fe{sub 2}O{sub 3} particles that exhibit the superparamagnetic behavior. It was established that the magnetic properties of nanoparticles significantly change with a decrease in their size to ∼6 nm. According to high-resolution electron microscopy and Mőssbauer spectroscopy data, the particle structure can be attributed to the ε–modification of trivalent iron oxide; meanwhile, the temperature of the magnetic order onset in these particles is increased, the well-known magnetic transition in the range of 80–150 K does not occur, the crystallographic magnetic anisotropy constant is significantly reduced, and the surface magnetic anisotropy plays a decisive role. This is apparently due to redistribution of cations over crystallographic positions with decreasing particle size, which was established using Mössbauer spectra. As the particle size is decreased and the fraction of surface atoms is increased, the contribution of an additional magnetic subsystem formed in a shell of particles smaller than ∼4 nm becomes significant, which manifests itself in the static magnetic measurements as paramagnetic contribution.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2017

Three-dimensional magnetic interactions in quasi-two-dimensional PdAs 2 O 6

Millimeter-sized PdAs 2 O 6 single crystals are grown using the vapor transport technique. The magnetic order at T N = 140 K is studied by measuring magnetic properties, specific heat, and neutron single crystal diffraction. The anisotropic magnetic susceptibility and a metamagnetic transition observed in magnetic fields above 20 kOe suggest that the magnetic moment lies in the ab plane, consistent with the magnetic structure determined by neutron single crystal diffraction. Below 140 K, Pd 2+ ions order ferromagnetically in the ab plane but antiferromagnetically along the crystallographic c axis. The ordered moment is refined to be 2.09(2) μ B /Pd 2+ using the fitted magnetic form factor of Pd 2+ . A weak λ-type anomaly around T N was observed in specific heat and the magnetic entropy change across T N is 1.72 J mol -1 K. This small entropy change and the temperature dependence of the magnetic susceptibility support the presence of short range correlations in a wide temperature range T N 2 O 6 suggests that the magnetic interactions in PdAs 2 O 6 are dominated by Pd-(O-$As\atop{As}$-O)-Pd super-superexchange and three dimensional despite the quasi-two-dimensional arrangement of magnetic ions. Finally, the comparison with NiAs 2 O 6 suggests that increasing covalency of isostructural compounds is an effective approach to design and to discover new materials with higher magnetic order temperatures in the localized regime.

36 MATERIALS SCIENCE↗