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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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DOE OSTI2021

Strong Magnetocrystalline Anisotropy Arising from Metal–Ligand Covalency in a Metal–Organic Candidate for 2D Magnetic Order

Layered metal–organic frameworks are promising candidates for new two-dimensional magnets, as their synthetic programmability of these materials can provide a route to diverse structural and electronic properties. However, such framework materials typically lack the heavy elements that engender magnetocrystalline anisotropy in the monolayer ferromagnets reported to date. Alternative sources of magnetic anisotropy are therefore needed in these materials. Here, we report the synthesis of single crystals of the framework material (NMe 4 ) 2 [Fe 2 L 3 ] (H 2 L = 3,6-dichloro-2,5-dihydroxybenzoquinone) and evaluate the angular dependence of its magnetic properties. Oriented-crystal magnetization measurements reveal strong uniaxial anisotropy, where the easy axis is aligned with the crystallographic c axis. While the spin carriers of this structure are isotropic $S = ^5/_2$ Fe III metal centers and $S = ^1/_2$ organic linkers, the anisotropy energy of the framework material is comparable to that of reported 2D ferromagnets. Density functional theory calculations indicate that the observed magnetocrystalline anisotropy arises from ligand-to-metal charge transfer that enhances the magnetic anisotropy of the otherwise isotropic Fe centers, suggesting that metal–ligand covalency can be utilized as a general additive for the development of 2D magnets. These results in this study show the possibility for (NMe 4 ) 2 [Fe 2 L 3 ] to retain magnetic order down to the 2D monolayer limit. In addition, the combination of large magnetic anisotropy and semiconducting character in (NMe 4 ) 2 [Fe 2 L 3 ] highlights its potential as a new 2D magnetic semiconductor.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Thermodynamics of emergent magnetic charge screening in artificial spin ice

Electric charge screening is a fundamental principle governing the behaviour in a variety of systems in nature. Through reconfiguration of the local environment, the Coulomb attraction between electric charges is decreased, leading, for example, to the creation of polaron states in solids or hydration shells around proteins in water. Here, we directly visualize the real-time creation and decay of screened magnetic charge configurations in a two-dimensional artificial spin ice system, the dipolar dice lattice. By comparing the temperature dependent occurrence of screened and unscreened emergent magnetic charge defects, we determine that screened magnetic charges are indeed a result of local energy reduction and appear as a transient minimum energy state before the system relaxes towards the predicted ground state. These results highlight the important role of emergent magnetic charges in artificial spin ice, giving rise to screened charge excitations and the emergence of exotic low-temperature configurations.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Out-of-plane chiral domain wall spin-structures in ultrathin in-plane magnets

Chiral spin textures in ultrathin films, such as skyrmions or chiral domain walls, are believed to offer large performance advantages in the development of novel spintronics technologies. While in-plane magnetized films have been studied extensively as media for current- and field-driven domain wall dynamics with applications in memory or logic devices, the stabilization of chiral spin textures in in-plane magnetized films has remained rare. Here we report a phase of spin structures in an in-plane magnetized ultrathin film system where out-of-plane spin orientations within domain walls are stable. Moreover, while domain walls in in-plane films are generally expected to be non-chiral, we show that right-handed spin rotations are strongly favoured in this system, due to the presence of the interfacial Dzyaloshinskii-Moriya interaction. These results constitute a platform to explore unconventional spin dynamics and topological phenomena that may enable high-performance in-plane spin-orbitronics devices.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Spin caloritronic nano-oscillator

Energy loss due to ohmic heating is a major bottleneck limiting down-scaling and speed of nano-electronic devices, and harvesting ohmic heat for signal processing is a major challenge in modern electronics. Here, we demonstrate that thermal gradients arising from ohmic heating can be utilized for excitation of coherent auto-oscillations of magnetization and for generation of tunable microwave signals. The heat-driven dynamics is observed in Y 3 Fe 5 O 12 /Pt bilayer nanowires where ohmic heating of the Pt layer results in injection of pure spin current into the Y 3 Fe 5 O 12 layer. This leads to excitation of auto-oscillations of the Y 3 Fe 5 O 12 magnetization and generation of coherent microwave radiation. Thus, our work paves the way towards spin caloritronic devices for microwave and magnonic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Generation of circularly polarized radiation from a compact plasma-based extreme ultraviolet light source for tabletop X-ray magnetic circular dichroism studies

Generation of circularly polarized light in the extreme ultraviolet (EUV) spectral region (about 25 eV–250 eV) is highly desirable for applications in spectroscopy and microscopy but very challenging to achieve in a small-scale laboratory. We present a compact apparatus for generation of linearly and circularly polarized EUV radiation from a gas-discharge plasma light source between 50 eV and 70 eV photon energy. In this spectral range, the 3p absorption edges of Fe (54 eV), Co (60 eV), and Ni (67 eV) offer a high magnetic contrast often employed for magneto-optical and electron spectroscopy as well as for magnetic imaging. We simulated and designed an instrument for generation of linearly and circularly polarized EUV radiation and performed polarimetric measurements of the degree of linear and circular polarization. Furthermore, we demonstrate first measurements of the X-ray magnetic circular dichroism at the Co 3p absorption edge with a plasma-based EUV light source. Our approach opens the door for laboratory-based, element-selective spectroscopy of magnetic materials and spectro-microscopy of ferromagnetic domains.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2017

Giant field-induced adiabatic temperature changes in In-based off-stoichiometric Heusler alloys

In this paper, direct measurements of the adiabatic temperature change (ΔT AD ) of Ni 50 Mn 35 In 14.5 B 0.5 have been done using an adiabatic magnetocalorimeter in a temperature range of 250–350 K, and with magnetic field changes up to ΔH = 1.8 T. The initial susceptibility in the low magnetic field region drastically increases with temperature starting at about 300 K. Magnetocaloric effects parameters, adiabatic temperature changes, and magnetic entropy changes were found to be a linear function of H 2/3 in the vicinity of the second order transitions (SOT), whereas the first order transitions do not obey the H 2/3 law due to the discontinuity of the transition. The relative cooling power based on the adiabatic temperature change for a magnetic field change of 1.8 T has been estimated. Maximum values of ΔT AD = -2.6 K and 1.7 K were observed at the magnetostructural transition (MST) and SOT for ΔH = 1.8 T, respectively. Finally, the observed ΔT AD at the MST exceeds the ΔT AD for Ni 50 Mn 35 In 14 X with X = In, Al, and Ge by more than 20% and is larger than the Gd based Heusler alloys.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Ferromagnetic response of multiferroic TbMnO{sub 3} films mediated by epitaxial strain and chemical pressure

High quality Tb{sub 1−x}Al{sub x}MnO{sub 3} (x = 0, 0.3) films have been grown under different values of compressive/tensile strain using (001)-oriented SrTiO{sub 3} and MgO substrates. The films were grown by means of rf sputtering at substrate temperature of 800 °C. X-ray diffraction analysis shows that films are single phase, preferentially oriented in the (111) and (122) directions for films deposited on SrTiO{sub 3} and MgO substrates, respectively. Although the TbMnO{sub 3} target shows antiferromagnetic order, the films deposited on both substrates show weak ferromagnetic phase at low temperature coexisting with the antiferromagnetic phase. The introduction of Al in the films clearly enhances their ferromagnetic behavior, improving the magnetic performance of this material. Indeed, M(H) measurements at 5 K show a well-defined hysteresis for films grown on both substrates. However, a stronger magnetic signal (larger values of remanence and coercive field) is observed for films deposited on MgO substrates. The chemical pressure generated by Al doping together with the substrate-induced strain seem to modify the subtle competition between magnetic interactions in the system. It is speculated that such modification could lead to a non-collinear magnetic state that may be tuned by strain modifications. This may be performed by varying the thickness of the films and/or considering other substrate materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Electrically controlled spin polarization and selection in a topological insulator sandwiched between ferromagnetic electrodes

We theoretically investigate the electrically controllable spin polarization and selective efficiency of the edge state Dirac electron in a two-dimensional topological insulator (TI) sandwiched between ferromagnetic (FM) electrodes by using the method of Keldysh nonequilibrium Green's function. A nearly full spin polarization of the topological edge state with giant inversion of ∼80% is observed, which is much higher than the value previously reported. Moreover, the selective efficiency for spin-up electrons under the modulation of the parallel configuration of FM electrodes has been demonstrated to be larger than 95% for the first time, while that for spin-down electrons in the antiparallel case is higher than 90% in a wide energy range, owing to the inter-edge spin tunneling induced backscattering and spin dephasing effect. The obtained results may provide a deeper understanding of the TI edge states and a valuable guidance to design spin switch and filter with high on-off speed and selective efficiency based on TIs.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Microstructure and phase composition characterization in a Co{sub 38}Ni{sub 33}Al{sub 29} ferromagnetic shape memory alloy

Transmission electron microscopy was performed to investigate the microstructures of a secondary phase and its surrounding matrix in a Co{sub 38}Ni{sub 33}Al{sub 29} ferromagnetic shape memory alloy. The secondary phase shows a γ′ L1{sub 2} structure exhibiting a dendritic morphology with enclosed B2 austenite regions while the matrix shows the L1{sub 0} martensitic structure. A secondary phase-austenite-martensite sandwich structure with residual austenite ranging from several hundred nanometers to several micrometers wide is observed at the secondary phase-martensite interface due to the depletion of Co and enrichment of Al in the chemical gradient zone and the effect of the strong martensitic start temperature dependency of the element concentrations. The crystallographic orientation relationship of the secondary phase and the B2 austenite fits the Kurdjumov-Sachs relationship. - Highlights: •The secondary phase has a γ′ L1{sub 2} structure exhibiting a dendritic morphology. •A secondary phase-austenite-martensite sandwich structure is observed. •The structural sandwich structure is due to elemental composition variation. •The secondary phase and the B2 austenite fit the Kurdjumov-Sachs relationship.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Magnetization distribution in Cu 0.6 Mn 2.4 Ge 2 ferromagnet from polarized and non-polarized neutron powder diffraction aided by density-functional theory calculations

The crystal structure and magnetic properties of Cu 0.6 Mn 2.4 Ge 2 have been re-investigated by a combination of extensive magnetic measurements and neutron scattering experiments, aided by electronic structure calculations. The material is found to be a soft ferromagnet with the ordering temperature T C = 316 K. The magnetocaloric effect evaluated from field-dependent magnetization isotherms is equal to 1.2 J/(kg·K) and 2.5 J/(kg·K) under the maximum applied magnetic field of 2 T and 5 T, respectively. The compound crystallizes in the hexagonal space group P6 3 /mmc. A complex structural disorder necessitated testing of several disorder models against the results of non-polarized and polarized neutron scattering experiments and magnetization measurements. Simulations at the density-functional theory level were also performed to identify the most robust solution that properly described the data observed. The final magnetic structure model reveals non-equal magnetic moments on the Mn1 and Mn2 atoms (2.29(9) µ B and 2.7(1) µ B , respectively) and the presence of vacancies and minor Cu substitution defects in both Mn sites. The work demonstrates how the non-polarized and polarized neutron scattering methods can be combined with electronic structure calculations to establish the microscopic structure of magnetic materials with complex crystallographic disorder.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Structural phase transition, narrow band gap, and room-temperature ferromagnetism in [KNbO{sub 3}]{sub 1−x}[BaNi{sub 1/2}Nb{sub 1/2}O{sub 3−δ}]{sub x} ferroelectrics

Structural phase transition, narrow band gap (E{sub g}), and room-temperature ferromagnetism (RTFM) have been observed in the [KNbO{sub 3}]{sub 1−x}[BaNi{sub 1/2}Nb{sub 1/2}O{sub 3−δ}]{sub x} (KBNNO) ceramics. All the samples have single phase perovskite structure, but exhibit a gradual transition behaviour from the orthorhombic to a cubic structure with the increase of x. Raman spectroscopy analysis not only corroborates this doping-induced change in normal structure but also shows the local crystal symmetry for x ≥ 0.1 compositions to deviate from the idealized cubic perovskite structure. A possible mechanism for the observed specific changes in lattice structure is discussed. Moreover, it is noted that KBNNO with compositions x = 0.1–0.3 have quite narrow E{sub g} of below 1.5 eV, much smaller than the 3.2 eV band gap of parent KNbO{sub 3} (KNO), which is due to the increasing Ni 3d electronic states within the gap of KNO. Furthermore, the KBNNO materials present RTFM near a tetragonal to cubic phase boundary. With increasing x from 0 to 0.3, the magnetism of the samples develops from diamagnetism to ferromagnetism and paramagnetism, originating from the ferromagnetic–antiferromagnetic competition. These results are helpful in the deeper understanding of phase transitions, band gap tunability, and magnetism variations in perovskite oxides and show the potential role, such materials can play, in perovskite solar cells and multiferroic applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Synthesis, Structural, Electronic, and Magnetic Properties of Cubic Perovskite La{sub 1−x}Ba{sub x}MnO{sub 3} (0.125 ≤ x ≤ 0.875) for Spintronic Devices

In this study, La{sub 0.5}Ba{sub 0.5}MnO{sub 3} has been synthesized by hydrothermal method. Crystal structure and morphology are determined by x-ray diffraction and scanning electron microscopy. It is observed that Ba-doped LaMnO{sub 3} (LMO) has the same cubic crystal structure as the host material with space group Pm3̄m. Half of the La atoms are replaced by Ba in the composition. Further, the electronic and magnetic structures are investigated by solving the Kohn-Sham equation with the full-potential linearized augmented plane wave method (FP-LAPW), with GGA+U approximation for exchange and correlation, for Ba concentration from 12.5 to 87.5%. The system is half-metallic ferromagnetic (FM) up to 55% and then converts into anti-ferromagnetic (AFM). This happens due to the onset of super exchange on increasing Ba concentrations. It is suggested that Ba-doped LMO is the best material for the fabrication of an exchange-biased spin valve. The spacer material can be any non-magnetic cubic perovskite such as BaTiO{sub 3} while the FM and AFM layers can be made of Ba-doped LMO with different concentrations of Ba. .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Monolayer 1T-LaN 2 : Dirac spin-gapless semiconductor of p -state and Chern insulator with a high Chern number

Two-dimensional transition-metal dinitrides have attracted considerable attention in recent years due to their rich magnetic properties. Here, we focus on rare-earth-metal elements and propose a monolayer of lanthanum dinitride with a 1T structural phase, 1T-LaN 2 . Using first-principles calculations, we systematically investigated the structure, stability, magnetism, and band structure of this material. It is a flexible and stable monolayer exhibiting a low lattice thermal conductivity, which is promising for future thermoelectric devices. Here, the monolayer shows the ferromagnetic ground state with a spin-polarized band structure. Two linear spin-polarized bands cross at the Fermi level forming a Dirac point, which is formed by the p atomic orbitals of the N atoms, indicating that monolayer 1T-LaN 2 is a Dirac spin-gapless semiconductor of p-state. When the spin–orbit coupling is taken into account, a large nontrivial indirect bandgap (86/354 meV) can be opened at the Dirac point, and three chiral edge states are obtained, corresponding to a high Chern number of C = 3, implying that monolayer 1T-LaN 2 is a Chern insulator. Importantly, this kind of band structure is expected to occur in more monolayers of rare-earth-metal dinitride with a 1T structural phase.

2D materials↗
DOE OSTI2015

Room temperature long range ferromagnetic ordering in Ni{sub 0.58}Zn{sub 0.42}Co{sub 0.10}Cu{sub 0.10}Fe{sub 1.8}O{sub 4} nano magnetic system

The structural and magnetic behavior of sol-gel autocombustion synthesized nanocrystalline Ni{sub 0.58}Zn{sub 0.42}Co{sub 0.10}Cu{sub 0.10}Fe{sub 1.8}O{sub 4} have been investigated by X-ray diffraction (XRD), transmission electron microscopy (TEM), Mössbauer spectroscopy and vibrating sample magnetometer(VSM). Sample of high purity and high homogeneity was obtained by calcination at low temperature (500°C) resulting in nanoparticles of average diameter ∼15nm as determined by XRD and further confirmed by TEM. X-ray diffraction (XRD) and selective area diffraction (SAED) confirmed the single phase of the sample. Mössbauer results are supported by magnetization data. Well defined sextets and appearance of hysteresis at room temperature indicate the existence of ferromagnetic coupling at room temperature finding material utility in magnetic storage data. The existence of iron in ferric state confirmed by isomer shift is a clear evidence of improved magnetic properties of the present system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Local geometric and electronic structures and origin of magnetism in Co-doped BaTiO{sub 3} multiferroics

We have prepared polycrystalline samples BaTi{sub 1−x}Co{sub x}O{sub 3} (x = 0–0.1) by solid-state reaction. X-ray diffraction and Raman-scattering studies reveal the phase separation in crystal structure as changing Co-doping content (x). The samples with x = 0–0.01 are single phase in a tetragonal structure. At higher doping contents (x > 0.01), there is the formation and development of a secondary hexagonal phase. Magnetization measurements at room temperature indicate a coexistence of paramagnetic and weak-ferromagnetic behaviors in BaTi{sub 1−x}Co{sub x}O{sub 3} samples with x > 0, while pure BaTiO{sub 3} is diamagnetic. Both these properties increase with increasing x. Analyses of X-ray absorption spectra recorded from BaTi{sub 1−x}Co{sub x}O{sub 3} for the Co and Ti K-edges indicate the presence of Co{sup 2+} and Co{sup 3+} ions. They locate in the Ti{sup 4+} site of the tetragonal and hexagonal BaTiO{sub 3} structures. Particularly, there is a shift of oxidation state from Co{sup 2+} to Co{sup 3+} when Co-doping content increases. We believe that the paramagnetic nature in BaTi{sub 1−x}Co{sub x}O{sub 3} samples is due to isolated Co{sup 2+} and Co{sup 3+} centers. The addition of Co{sup 3+} ions enhances the paramagnetic behavior. Meanwhile, the origin of ferromagnetism is due to lattice defects, which is less influenced by the changes caused by the variation in concentration of Co{sup 2+} and Co{sup 3+} ions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Studies on magnetic properties of chemically synthesized crystalline calcium ferrite nanoparticles

Spinel-type ferrites have taken a very important role for modern electronic industry. Most of these ferrites exhibit low-loss dielectric properties, high resistivity, low eddy current and also high temperature ferromagnetism. Calcium ferrite is one such important metal oxide which is environmentally safe, chemically stable, low cost and greatly abundant. This outstanding material of calcium ferrite is synthesized by a simple chemical precipitation method using NaOH as the precipitating agent. Ferric chloride anhydrous (FeCl{sub 3}) and Calcium chloride dihydrate (CaCl{sub 2}.2H{sub 2}O) were used as iron and calcium sources respectively. The samples were heated at 200°C for 8h to obtain homogeneous powder of Calcium ferrite. The powders were characterized by using X-ray diffraction (XRD), field emission scanning electron microscope (FESEM), Transmission electrical microscopy (TEM), and Fourier transform infrared spectroscopic (FTIR) measurements. The polycrystalline nature of the sample was confirmed by X-ray diffraction study. The magnetic properties of the sample were investigated by vibrating sample magnetometer (VSM) measurements. Magnetization curve of the prepared sample depicts that as synthesized calcium ferrite nanoparticles have saturation magnetic moment of 1.74 emu/g and the coercivity of 35.08 Oe with superparamagnetic behavior. The synthesized calcium ferrite nanoparticles with such magnetic properties will be a candidate material for different applications in electronics and exploring its functionality in the field of recently developing semiconductor device physics and spintronics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2021

Switching of a Magnet by Spin-Orbit Torque from a Topological Dirac Semimetal

Recent experiments show that topological surface states (TSS) in topological insulators (TI) can be exploited to manipulate magnetic ordering in ferromagnets. In principle, TSS should also exist for other topological materials, but it remains unexplored as to whether such states can also be utilized to manipulate ferromagnets. In this paper, current-induced magnetization switching enabled by TSS in a non-TI topological material, namely, a topological Dirac semimetal α-Sn, is reported. The experiments use an α-Sn/Ag/CoFeB trilayer structure. The magnetization in the CoFeB layer can be switched by a charge current at room temperature, without an external magnetic field. The data show that the switching is driven by the TSS of the α-Sn layer, rather than spin-orbit coupling in the bulk of the α-Sn layer or current-produced heating. The switching efficiency is as high as in TI systems. This shows that the topological Dirac semimetal α-Sn is as promising as TI materials in terms of spintronic applications.

36 MATERIALS SCIENCE↗
DOE OSTI2017

A Model Study of Substrate Effect on the Neutron-Scattering Spectra of Ferromagnetic Ordered Graphene

Graphene as a possible new magnetic material has stimulated research interest for application in spintronic devices. Pristine graphene does not show magnetism due to equivalence of the two sub-lattices of carbon atoms. It is predicted that impurity effects, substrate-induced gap, and defects, are expected to produce in-equivalence in two carbon sub-lattices leading to magnetism. The spins on the same sub-lattices are found to exhibit ferromagnetic order and spins of different sub-lattices are found to exhibit anti-ferromagnetic order. We consider here impurity and substrate effects as the cause of generation of magnetism in graphene. We report here a microscopic tight-binding study of frequency-dependent neutron scattering spectra for ferromagnetic ordering in the graphene systems. The tight-binding Hamiltonian consists of electron hoppings upto third nearest neighbors and substrate and impurity effects in the presence of Coulomb interaction of electrons separately at two in-equivalent A and B sub-lattices of graphene. We calculate the two-particle electron Green’s functions by using Zubarev’s Green’s function technique. The frequency-dependent scattering intensity of the system is computed numerically. The spectra displays a sharp peak at the neutron momentum transfer energy at low energies and another higher-energy peak appearing at substrate-induced gap.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗