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DOE OSTI2022

Statistics on magnetic properties of Co compounds: A database-driven method for discovering Co-based ferromagnets

The search for new ferromagnetic compounds is often targeted at known structure families, particularly those containing iron, cobalt, and manganese. Here, we propose a method to expand this search to lesser-known structure types, using a database of experimental Curie and Néel temperatures. This study, in particular, illustrates the case of compounds containing the element cobalt, and we demonstrate how the use of such a database can lead to the discovery of ferromagnetic materials that had previously been overlooked. We report statistics from a literature survey of the magnetic properties of Co-based compounds with more than 33 at. % Co. We classify more than 13 000 compounds by structure type, cobalt content, and magnetic ground state. From these data, compounds TaCo 2 Ga, La 6 Co 13 Bi, and Nd 2 Co 3 were identified as potential ferromagnets, and we confirm their ferromagnetic ordering theoretically via first-principles calculations and experimentally via synthesis and characterization measurements. In addition, the analysis is focused on the collection of data trends and discovery of ferromagnetic materials with easy-axis magnetic anisotropy. Both known ferromagnetic materials with unknown magnetic anisotropy, and unstudied compounds were considered. From the subset of known ferromagnets with unknown anisotropy, the compound Co 2 Mg was synthesized, characterized, and determined to have easy-axis magnetic anisotropy at room temperature.

36 MATERIALS SCIENCE↗

NASA NTRS1982

Photovoltaic properties of ferroelectric BaTiO3 thin films RF sputter deposited on silicon

Ferroelectric thin films of BaTiO3 have been successfully deposited on n-type silicon substrates at temperatures above 500 C by RF sputtering in an O2/Ar atmosphere. Analysis by X-ray diffraction patterns show that films deposited at room temperature are amorphous. At temperatures above 500 C, crystalline BaTiO3 films with a tetragonal structure are obtained. The polarization-electric field (P-E) hysteresis loops and a broad peak in the dielectric constant versus temperature curve at Curie point indicate that the RF sputtered BaTiO3 films are ferroelectric. An anomalous photovoltaic effect is observed in these thin films which is related to the remanent polarization of the material. The results on open-circuit and short-circuit measurements provide an important basis for a better understanding of the role of photovoltaic field, photovoltaic current, and the pyroelectric properties in photoferroelectric domain switching.

Dharmadhikari, V. S.↗

NASA NTRS1988

Remanent magnetism at Mars

It is shown that a strong case can be made for an intrinsic magnetic field of dynamo origin for Mars earlier in its history. The typical equatorial magnetic field intensity would have been equal to about 0.01-0.1 gauss. The earlier dynamo activity is no longer extant, but a significant remanent magnetic field may exist. A highly non-dipole magnetic field could result from the remanent magnetization of the surface. Remanent magnetization may thus play an important role in the Mars solar wind interactions, in contrast to Venus with its surface temperatures above the Curie point. The anomalous characteristics of Mars'solar wind interaction compared to that of Venus may be explicable on this basis.

Curtis, S. A.↗

DOE OSTI2020

Ferromagnetic cluster-glass phase in Ca(Co 1-x Ir x ) 2-y As 2 crystals

In this study, single crystals of Ca(Co 1-x Ir x ) 2-y As 2 with 0≤x≤0.35 and 0.10≤y≤0.14 have been grown using the self-flux technique and characterized by single-crystal x-ray diffraction (XRD), energy-dispersive x-ray spectroscopy, magnetization M, and magnetic susceptibility χ measurements versus temperature T, magnetic field H, and time t, and heat-capacity C p (H,T) measurements. The XRD refinements reveal that all the Ir-substituted crystals crystallize in a collapsed-tetragonal structure as does the parent CaCo 2-y As 2 compound. A small 3.3% Ir substitution for Co in CaCo 1.86 As 2 drastically lowers the A-type antiferromagnetic (AFM) transition temperature T N from 52 to 23 K with a significant enhancement of the Sommerfeld electronic heat-capacity coefficient. The A-type AFM structure consists of ab-plane layers of spins ferromagnetically aligned along the c axis with AFM alignment of the spins in adjacent layers along this axis. The positive Weiss temperatures obtained from Curie-Weiss fits to the χ(T>T N ) data indicate that the dominant magnetic interactions are ferromagnetic (FM) for all x. A magnetic phase boundary is inferred to be present between x=0.14 and x=0.17 from a discontinuity in the x dependencies of the effective moment and Weiss temperature in the Curie-Weiss fits. FM fluctuations that strongly increase with increasing x are also revealed from the χ(T) data. Furthermore, the magnetic ground state for x≥0.17 is a spin glass as indicated by hysteresis in χ(T) between field-cooled and zero-field-cooled measurements and from the relaxation of M in a small field that exhibits a stretched-exponential time dependence. The spin glass has a small FM component to the ordering and is hence inferred to be comprised of small FM clusters. The competing AFM and FM interactions along with crystallographic disorder associated with Ir substitution are inferred to be responsible for the development of a FM cluster-glass phase. A logarithmic T dependence of Cp at low T for x=0.14 is consistent with the presence of significant FM quantum fluctuations. This composition is near the T=0 boundary at x≈0.16 between the A-type AFM phase containing ferromagnetically-aligned layers of spins and the FM cluster-glass phase.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1976

Magnetic heat pumping near room temperature

It is shown that magnetic heat pumping can be made practical at room temperature by using a ferromagnetic material with a Curie point at or near operating temperature and an appropriate regenerative thermodynamic cycle. Measurements are performed which show that gadolinium is a resonable working material and it is found that the application of a 7-T magnetic field to gadolinium at the Curie point (293 K) causes a heat release of 4 kJ/kg under isothermal conditions or a temperature rise of 14 K under adiabatic conditions. A regeneration technique can be used to lift the load of the lattice and electronic heat capacities off the magnetic system in order to span a reasonable temperature difference and to pump as much entropy per cycle as possible

Brown, G. V.↗

DOE OSTI2024

Large adiabatic temperature change and magnetic frustration in triangular lattice antiferromagnet Dy 2 IrSi 3

While previous studies reveal that the formation of polycrystalline R 2 TX 3 (R = rare-earth, T = transition metal, X = p-block element) type compounds with T = Ir and Co is not achievable without deliberate introduction of atomic vacancies of Ir/Co and Si, here we report successful synthesis of Dy 2 IrSi 3 with fully stoichiometric ratio of constituent elements. An antiferromagnetic transition is manifested in the compound at 6.6 K where only about 50 % of Dy spins take part, while the rest remain in highly frustrated state due to edge-sharing triangular lattice geometry. The magnetic frustration is conclusively probed through magnetization, heat capacity and magnetocaloric study and the frustration parameter (f = |θ p |/T N , θ p , T N being Curie-Weiss and Néel temperatures, respectively) in this case is as large as ~ 3. An additional cluster-glass type transition at ~2.8 K observed in this system has likely been originated due to this magnetic frustration. The magnetocaloric effect reveals an adiabatic temperature change of ~7.5 K for 70 kOe magnetic field, which is one of the largest values reported in intermetallic compounds.

36 MATERIALS SCIENCE↗

NASA NTRS1982

Measurements of the lunar induced magnetic moment in the geomagnetic tail - Evidence for a lunar core

Apollo 15 and 16 subsatellite fluxgate magnetometer data have been analyzed for all intervals in which the moon was in the lobes of the geomagnetic tail to obtain an improved estimate of the average magnitude of the induced dipole moment of the moon. The resulting set of estimates yields an induced magnetic moment of -4.23 x 10 to the 22nd Gauss-cu cm per Gauss of applied field, corresponding to a G-factor of -0.008 + or - 0.001. These measurements do not place strong constraints on the conductivity of the lunar core. The observed effects would be detected as long as the core conductivity was greater than about 10 mho/m. If the outer cool layers of the moon that are at temperatures below the effective Curie point contain little or no free iron, then these measurements are consistent with the presence of a conducting core whose radius is slightly larger than 400 km. If these outer layers of the moon contain significant amounts of free iron and hence exhibit the paramagnetism expected in such a situation the core size could be even greater.

Russell, C. T.↗

NASA NTRS1987

Electron-Spin Resonance in Boron Carbide

Samples exhibit Curie-law behavior in temperature range of 2 to 100 K. Technical paper presents studies of electron-spin resonance of samples of hot pressed B9 C, B15 C2, B13 C2, and B4 C. Boron carbide ceramics are refractory solids with high melting temperatures, low thermal conductives, and extreme hardnesses. They show promise as semiconductors at high temperatures and have unusually large figures of merit for use in thermoelectric generators.

Wood, Charles↗

NASA NTRS2005

Novel Applications of Magnetic Fields for Fluid Flow Control and for Simulating Variable Gravity Conditions

Static and dynamic magnetic fields have been used to control convection in many materials processing applications. In most of the applications, convection control (damping or enhancement) is achieved through the Lorentz force that can be tailored to counteract/assist dominant system flows. This technique has been successfully applied to liquids that are electrically conducting, such as high temperature melts of semiconductors, metals and alloys, etc. In liquids with low electrical conductivity such as ionic solutions of salts in water, the Lorentz force is weak and hence not very effective and alternate ways of flow control are necessary. If the salt in solution is paramagnetic then the variation of magnetic susceptibility with temperature and/or concentration can be used for flow control. For thermal buoyancy driven flows this can be accomplished in a temperature range below the Curie point of the salt. The magnetic force is proportional to the magnetic susceptibility and the product of the magnetic field and its gradient. By suitably positioning the experiment cell in the magnet, system flows can be assisted or countered, as desired. A similar approach can be extended to diamagnetic substances and fluids but the required magnetic force is considerably larger than that required for paramagnetic substances. The presentation will provide an overview of work to date on a NASA fluid physics sponsored project that aims to test the hypothesis of convective flow control using strong magnetic fields in protein crystal growth. The objective is to understand the nature of the various forces that come into play, delineate causative factors for fluid flow and to quantify them through experiments, analysis, and numerical modeling. The seminar will report specifically on the experimental results using paramagnetic salts and solutions in magnetic fields and compare them to analytical predictions. Applications of the concept to protein crystallization studies will be discussed. The use of strong magnetic fields for terrestrially simulating variable gravity environments and applications supporting the NASA Exploration Initiative will also be briefly discussed.

Ramachandran, N.↗

DOE OSTI2022

Electronic and magnetic properties of the topological semimetal SmMg 2 Bi 2

Dirac semimetals show nontrivial physical properties and can host exotic quantum states like Weyl semimetals and topological insulators under suitable external conditions. Here, by combining angle-resolved photoemission spectroscopy measurements (ARPES) and first-principle calculations, we demonstrate that the Zintl-phase compound SmMg 2 Bi 2 is in close proximity to a topological Dirac semimetallic state. ARPES results show a Dirac-like band crossing at the zone center near the Fermi level (E F ), which is further confirmed by first-principle calculations. Theoretical studies also reveal that SmMg 2 Bi 2 belongs to a Z 2 topological class and hosts spin-polarized states around the E F . Zintl's theory predicts that the valence state of Sm in this material should be Sm 2+ , however, we detect many Sm-4f multiplet states (flat-bands) whose energy positions and relative intensities suggest the presence of both dominant Sm 2+ and minor Sm 3+ . The small concentration (2.5%) of Sm 3+ in the bulk of a crystal is inferred to arise from Sm vacancies in the crystal. It is also evident that these flat bands and other dispersive states are strongly hybridized when they cross each other. Due to the presence of Sm 3+ ions, the temperature dependence of the magnetic susceptibility χ (T) shows a Curie-Weiss-like contribution in the low-temperature region, in addition to the Van Vleck-like behavior expected for the Sm 2+ ions. The present study will help to better understand the electronic structure, magnetism, and transport properties of related materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Paramagnetic Properties of Rare Earth Hydroxides, Oxalates, and Dibutyl Phosphates

Magnetic separations present a promising approach for the recovery of rare earth (RE) elements from mixtures, particularly when coupled with precipitation techniques that enhance process efficiency and selectivity. However, the magnetic properties of RE materials typically encountered in the separations industry are not well characterized. Here, we synthesized a series of RE materials, combining four REs – praseodymium (Pr), neodymium (Nd), terbium (Tb), and dysprosium (Dy) – with three precipitating agents – hydroxide, oxalate, and dibutyl phosphate. All materials showed typical paramagnetic behavior consistent with the Curie-Weiss law. At low temperatures, we observed weak antiferromagnetic correlations, which were more pronounced for the lighter RE ions (Pr, Nd). Particle morphology and crystallography analyses showed that the dibutyl phosphates were well-ordered metal-organic frameworks, the oxalates were crystals with mixed hydration states, and the hydroxides were mostly amorphous. Regardless of the degree of crystallinity, the effective magnetic moments aligned well with theoretical estimates based on Hund's rules and 4f electron configurations of the corresponding RE ions. For a given RE ion, the magnetophoretic response was thus determined by the size of the particles rather than specific metal-ligand coupling, with dibutyl phosphate promoting the formation of larger crystals that were the most strongly attracted to magnets.

Wang, Qingpu (ORCID:0000000156041571)↗

DOE OSTI2020

Supramolecular Assembly of U(IV) Clusters and Superatoms with Unconventional Countercations

Superatoms are nanometer-sized molecules or particles that form ordered lattices, mimicking their atomic counterparts. Hierarchical assembly of superatoms gives rise to emergent properties in lattices of quantum dots, p-block clusters, and fullerenes. In this report, we introduce a family of uranium-oxysulfate cluster anions whose hierarchical assembly in water is controlled by two parameters: acidity and the lanthanide or transition-metal countercation. In acid, larger Ln III (Ln = La–Ho) link hexamer (U 6 ) oxoclusters into body-centered cubic frameworks, while smaller Ln III (Ln = Er–Lu and Y) promote linking of 14 U 6 clusters into hollow superclusters (U 84 superatoms). U 84 assembles into superlattices including cubic-closest packed, body-centered cubic, and interpenetrating networks, bridged by interstitial countercations and U 6 clusters. Divalent transition metals (TM = Mn II and Zn II ) charge-balance and promote the fusion of 10 U 6 and 10 U monomers into a wheel-shaped cluster (U 70 ). Dissolution of U 70 in organic media shows (by small-angle X-ray scattering) that differing supramolecular assemblies are accessed, controlled by TM II -linking of U 70 clusters. Magnetic measurements of these assemblies reveal Curie–Weiss behavior at high temperatures, without pairing of the 5f 2 -electrons down to 2 K.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Physical properties of YbFe 5 P 3 with a quasi-one-dimensional crystal structure

We report basic physical properties of the quasi-one-dimensional heavy-fermion compound Yb Fe 5 P 3 . Its magnetic susceptibility follows a modified Curie-Weiss behavior at high temperatures with a Weiss temperature between - 5 and - 21 K depending on the direction of the applied magnetic field. Our single crystals of Yb Fe 5 P 3 are good metals with a room-temperature resistivity of ~ 140 μ Ω cm and a residual resistivity of less than 2 μ Ω cm. Below ~ 2 K the resistivity reflects the presence of strong quantum fluctuations, which is supported by specific heat measurements that show a similar strong enhancement in C / T at low temperatures reaching 1.5 J/mol K 2 below T = 0.5 K. No magnetic ordering is observed down to 80 mK. Magnetic fields up to 8 T rapidly suppress the magnetic fluctuations, while resistivity measurements under pressures up to 2.54 GPa indicate the enhancement of quantum fluctuations, although still no order is observed down to 0.3 K. Density functional theory calculations suggest the presence of electronically quasi-one-dimensional (1D) Fermi surface sheets together with three-dimensional electronic pockets. We suggest that the quasi-1D nature of this compound leads to an extended regime of large quantum fluctuations within the paramagnetic state prior to reaching a magnetic instability.

36 MATERIALS SCIENCE↗

NASA NTRS1972

Thermodynamics of the Heisenberg ferromagnet in an applied magnetic field.

The anisotropic-Heisenberg-ferromagnet formalism developed previously is examined to include an applied magnetic field for the isotropic case in the random-phase approximation. Thermodynamic quantities such as magnetization, susceptibility, and the derivative of magnetization with respect to temperature are studied near the Curie point.

Flax, L.↗

NASA NTRS2006

Fast Erase Method and Apparatus For Digital Media

A non-contact fast erase method for erasing information stored on a magnetic or optical media. The magnetic media element includes a magnetic surface affixed to a toroidal conductor and stores information in a magnetic polarization pattern. The fast erase method includes applying an alternating current to a planar inductive element positioned near the toroidal conductor, inducing an alternating current in the toroidal conductor, and heating the magnetic surface to a temperature that exceeds the Curie-point so that information stored on the magnetic media element is permanently erased. The optical disc element stores information in a plurality of locations being defined by pits and lands in a toroidal conductive layer. The fast erase method includes similarly inducing a plurality of currents in the optical media element conductive layer and melting a predetermined portion of the conductive layer so that the information stored on the optical medium is destroyed.

Oakely, Ernest C.↗

NASA NTRS2004

Magnetocaloric Pumping of Liquid Oxygen

The field-induced force density on a magnetic fluid is proportional to the magnetic susceptibility times the gradient of the magnetic field squared. The direction of the force is towards increasing magnetic field (positive gradient). Applying a magnetic field to a magnetic fluid will result in a force from all directions towards the location of peak field. Since the magnetic field is conservative and there are no magnetic monopoles, the net field-induced force on any fluid of constant susceptibly will be zero. The only manner to obtain a nonzero net field-induced force is to vary the susceptibility of the fluid. At the gas/liquid interface of liquid oxygen, the susceptibility varies drastically, and the exploitation of the resultant large net forces. An alternative method of varying the magnetic susceptibility is to vary the temperature of the fluid. The magnetic susceptibility of paramagnetic liquid oxygen obeys the Curie-Weiss law: it is inversely proportional to temperature. By applying a temperature gradient in the presence of a symmetric magnetic field, a nonzero net force results. Much of the theory of the so-called Magnetocaloric Effect has previously been developed for and applied to ferromagnetic fluids, or ferrofluids, but is readily applied to paramagnetic liquid oxygen.

Immer, Christopher↗

NASA NTRS1981

New magnetic results from Allende C3/V/

Thermomagnetic analyses of Allende C3(V) suggest that magnetic phases contributing about 15% to saturation magnetization with transition temperatures not greater than 320 C, also contribute about 90% to natural remanence (NRM) and about 80% to the saturation isothermal remanence (SIRM). Phases carrying the dominating part of of the NRM are found to be intergrown, magnetically interacting, and thermally unstable, beginning at temperatures as low as 50 C. The ratio of the NRM/SIRM ranges from 0.004 to 0.006 for the bulk meteorite and from 0.0004 to 0.005 for chondrules of all sizes. The remanent coercive force behavior suggests coexisting magnetic phases with differing Curie points or with the low temperature transitions being due to transformation of a thermally metastable phase.

Wasilewski, P.↗

DOE OSTI2026

Physical properties and anisotropic magnetism of EuBi 2

We report the synthesis of EuBi 2 single crystals and their magnetic and electronic properties. Plate-like crystals were grown in excess bismuth, and X-ray diffraction data confirm the previously reported tetragonal space group, I 4 1 /amd (No. 141). A Néel temperature of T N = 18.6 K was determined from the specific heat data, and corresponding anomalies occur in the magnetization and resistivity. We only observe one magnetic transition in zero magnetic field. The magnetization data above 70 K are well described by a Curie-Weiss model with a Weiss temperature of Θ CW ≈ −35 K and an effective moment near that of the expected spin-only moment of Eu 2+ (S = 7/2). Isothermal magnetization measurements reveal field-induced transitions for H||[100], including a hysteretic spin-flop centered at 10.1 T and a change in slope at 12 T and 2 K. However, while the isothermal magnetization for H||[110] displays nonlinear behavior, discrete metamagnetic transitions are not observed for H||[110] or H||[001], indicating significant magnetic anisotropy. The magnetization does not saturate by 13.5 T for any orientation. EuBi 2 is metallic and our crystals possess an in-plane residual resistivity ratio of ⍴300 K/⍴2 K ≈ 40. Single crystal neutron diffraction data reveal a large magnetic unit cell and non-trivial antiferromagnetic ordering. These results demonstrate that strong antiferromagnetic coupling drives complex magnetism in EuBi 2 .

36 MATERIALS SCIENCE↗