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At least 667 records · Page 37
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Strong Electronic and Magnetic Coupling in M 4 (M = Ni, Cu) Clusters via Direct Orbital Interactions between Low-Coordinate Metal Centers

In this report we present an extensive study of tetranuclear transition-metal cluster compounds M 4 (NP t Bu 3 ) 4 and [M 4 (NP t Bu 3 ) 4 ][B(C 6 F 5 ) 4 ] (M = Ni, Cu; t Bu = tert -butyl), which feature low-coordinate metal centers and direct metal-metal orbital overlap. X-ray diffraction, electrochemical, magnetic, spectroscopic, and computational analysis elucidate the nature of the bonding interactions in these clusters and the impact of these interactions on the electronic and magnetic properties. Direct orbital overlap results in strongly coupled, large-spin ground states in the [Ni 4 (NP t Bu 3 ) 4 ] +/0 clusters and fully delocalized, spin-correlated electrons. Correlated electronic structure calculations confirm the presence of ferromagnetic ground states that arise from direct exchange between magnetic orbitals, and, in the case of the neutral cluster, itinerant electron magnetism similar to that in metallic ferromagnets. The cationic nickel cluster also possesses large magnetic anisotropy exemplified by a large, positive axial zero-field splitting parameter of D = +7.95 or +9.2 cm -1 , as determined by magnetometry or electron paramagnetic resonance spectroscopy, respectively. The [Ni 4 (NP t Bu 3 ) 4 ] + cluster is also the first molecule with easy-plane magnetic anisotropy to exhibit zero-field slow magnetic relaxation, and under a small applied field, it exhibits relaxation exclusively through an Orbach mechanism with a spin relaxation barrier of 16 cm -1 . The S = 1 / 2 complex [Cu 4 (NP t Bu 3 ) 4 ] + exhibits slow magnetic relaxation via a Raman process on the millisecond time scale, supporting the presence of slow relaxation via an Orbach process in the nickel analogue. Overall, this work highlights the unique electronic and magnetic properties that can be realized in metal clusters featuring direct metal-metal orbital interactions between low-coordinate metal centers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Structural, magnetic, and dielectric studies of the Aurivillius compounds SrBi{sub 5}Ti{sub 4}MnO{sub 18} and SrBi{sub 5}Ti{sub 4}Mn{sub 0.5}Co{sub 0.5}O{sub 18}

We have successfully synthesized the Aurivillius compounds SrBi{sub 5}Ti{sub 4}MnO{sub 18} and SrBi{sub 5}Ti{sub 4}Mn{sub 0.5}Co{sub 0.5}O{sub 18} using a modified Pechini method. Both samples have an orthorhombic structure with the space group B2cb. The valence state of Mn is suggested to be +3 and the doped Co ions exist in the form of Co{sup 2+} and Co{sup 3+} based on the results of x-ray photoelectron spectroscopy. The sample SrBi{sub 5}Ti{sub 4}MnO{sub 18} exhibits a dominant paramagnetic state with the existence of superparamagnetic state as evidenced by the electron paramagnetic resonance results, whereas SrBi{sub 5}Ti{sub 4}Mn{sub 0.5}Co{sub 0.5}O{sub 18} undergoes a ferrimagnetic transition at 161 K originating from the antiferromagnetic coupling of Co-based and Mn-based sublattices, and a ferromagnetic transition at 45 K arising from the Mn{sup 3+}-O-Co{sup 3+} (low spin) interaction. The sample SrBi{sub 5}Ti{sub 4}Mn{sub 0.5}Co{sub 0.5}O{sub 18} exhibits two dielectric anomalies. One corresponds to a relaxor-like dielectric relaxation which follows the Vogel-Fulcher function and the other dielectric relaxation obeys the Arrhenius law arising from the collective motion of oxygen vacancies. In addition, the sample SrBi{sub 5}Ti{sub 4}Mn{sub 0.5}Co{sub 0.5}O{sub 18} exhibits a magnetodielectric effect caused by the Maxwell-Wagner effect because of the conductivity of the sample. This is demonstrated by the fact that the activation energy in dielectric loss process is close to that for dc conductivity and the magnetodielectric effect is sensitive to the measured frequency.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Specific Features of the Electron Spin Resonance of an Iron Impurity in HgSe Crystals

The electron-spin-resonance spectra of transition metal ions Fe in the HgSe matrix are analyzed. The spectra have an appearance typical of the Fe{sup 3+} ion, i.e., they consist of five fine-structure lines with a splitting that corresponds to a weak crystal field. The spectra are observed at temperatures of up to 50 K. The spectral lines are deformed and have a Dyson shape. An analysis of the temperature dependences of the line amplitudes shows that a transition from paramagnetic ordering to ferromagnetic ordering occurs with decreasing temperature, with the Curie temperature T ≈ 7 K.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Epitaxial stabilization of ultra thin films of electron doped manganites

Ultra-thin films of the electron doped manganite La{sub 0.8}Ce{sub 0.2}MnO{sub 3} were grown in a layer-by-layer growth mode on SrTiO{sub 3} (001) substrates by pulsed laser interval deposition. High structural quality and surface morphology were confirmed by a combination of synchrotron based x-ray diffraction and atomic force microscopy. Resonant X-ray absorption spectroscopy measurements confirm the presence of Ce{sup 4+} and Mn{sup 2+} ions. In addition, the electron doping signature was corroborated by Hall effect measurements. All grown films show a ferromagnetic ground state as revealed by both dc magnetization and x-ray magnetic circular dichroism measurements and remain insulating contrary to earlier reports of a metal-insulator transition. Our results hint at the possibility of electron-hole asymmetry in the colossal magnetoresistive manganite phase diagram akin to the high-T{sub c} cuprates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Disorder-driven phase transition in La{sub 0.37}D{sub 0.30}Ca{sub 0.33}MnO{sub 3} (D = Bi, Sm) manganites

In the present work we report the structural, electron spin resonance (ESR) and magnetic properties of La{sub 0.37}D{sub 0.30}Ca{sub 0.33}MnO{sub 3} (D = Bi, Sm) manganites synthesized by sol-gel method. The critical behavior at the critical point, where the system undergoes phase transition from paramagnetic (PM) to ferromagnetic (FM) state, is investigated by using modified-Arrott plots, Kouvel-Fisher method and critical isotherm analysis. Both the samples show second-order phase transition near the critical point. The decrease in magnetization (M), Curie temperature (T{sub C}), evolution of spin or cluster glass behavior and the nature of second-order phase transition compared to the first-order transition reported in the literature for La{sub 0.67}Ca{sub 0.33}MnO{sub 3} are ascribed to disorder caused by the size mismatch of the A-site cations with Bi and Sm doping at La-site.

36 MATERIALS SCIENCE↗
DOE OSTI2014

New opportunities in microwave electronics with ferromagnetic nanowires

A series of monolithic tunable microwave band-stop filters and phase shifters have been designed, fabricated, and characterized on arrays of ferromagnetic nanowires (FMNWs) constituted of Ni, Co, CoFeB, and NiFe alloy embedded in anodic alumina templates (AAO). The aim of the present investigation is to significantly boost the operating frequency of devices in very low applied magnetic field. The stop-band response can cover from 8 to 40 GHz with an applied magnetic field up to 5 kOe using these materials. In addition, we observed a substantial increase in frequency tunability (>110%) for Ni and NiFe alloy based filter. Frequency bandwidth/linewidth can be tuned with the proper choice of magnetic material, broad band for Co nanowires to narrow band for CoFeB nanowires. The amorphous nature of CoFeB reduces linewidth considerably and hence increases resonance absorption. It is also observed that the frequency linewidth (Δf) decreases with increasing applied magnetic field. The same filter can be used as a tunable phase shifter. For Ni nanowire based phase shifter, a maximum shift of 75°/cm at 4 kOe was observed.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Anomalous Antiferromagnetism in Metallic RuO 2 Determined by Resonant X-ray Scattering

We studied the magnetic ordering of thin films and bulk crystals of rutile RuO 2 using resonant X-ray scattering across the Ru L 2 absorption edge. Combining a polarization analysis and azimuthal-angle dependence of the magnetic Bragg signal, we have established the presence of G-type anti-ferromagnetism in RuO 2 with TN > 300 K. In addition to revealing a spin-ordered ground state in the simplest ruthenium oxide compound, the persistence of magnetic order even in nanometer-thick films lays the ground for potential applications of RuO 2 in antiferromagnetic spintronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

From Layered Antiferromagnet to 3D Ferromagnet: LiMnBi-to-MnBi Magneto-Structural Transformation

Here, the intermetallic compound LiMnBi was synthesized by the two-step solid-state reaction from the elements. The synthesis temperature of 850 K was selected based on in-situ high-temperature powder X-ray diffraction data. LiMnBi crystalizes in the layered-like PbClF structure type (a = 4.3131(7) Å, c = 7.096(1) Å at 100 K, P4/nmm space group, Z = 2). LiMnBi structure is built of the alternating [MnBi] and Li layers, as determined from single-crystal X-ray diffraction data. Magnetic properties measurements and solid-state 7 Li Nuclear Magnetic Resonance data collected for polycrystalline LiMnBi samples indicate the long-range antiferromagnetic ordering of Mn sublattice at ~340 K, with no superconductivity down to 5 K detected. LiMnBi is air- and water-sensitive. In aerobic conditions, Li can be extracted from LiMnBi structure to form Li 2 O/LiOH and MnBi (NiAs structure type, P6 3 /mmc). The obtained MnBi polymorph was previously reported to be one of the strongest rare-earth-free ferromagnets, yet its bulk synthesis in powder form is cumbersome. The proposed magneto-structural transformation from ternary LiMnBi to ferromagnetic MnBi involves condensation of the MnBi4 tetrahedra upon Li deintercalation and is exclusive to LiMnBi. In contrast, ferromagnetic MnBi cannot be obtained from either isostructural NaMnBi and KMnBi, or from the structurally related CaMn 2 Bi 2 . Such a distinctive transformation in the case of LiMnBi is presumed to be due to its fitting reactivity to yield MnBi and favorable interlayer distance between [MnBi] layers, while the interlayer distance in NaMnBi and KMnBi structural analogs is unfavorably long. The studies of delithiation from the layered-like LiMnBi under different chemical environments indicate that the yield of the MnBi depends on the type of solvent used and the kinetics of the reaction. A slow rate and mild reaction media lead to a high fraction of the MnBi product. The saturation magnetization of the “as-prepared” MnBi is ~50 % of the expected value of 81.3 emu/g. Overall, this study adds a missing member to the family of ternary pnictides and illustrates how soft-chemistry methods can be used to obtain “difficult-to-synthesize” compounds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Resonance from antiferromagnetic spin fluctuations for superconductivity in UTe 2

We report superconductivity originates from the formation of bound (Cooper) pairs of electrons that can move through the lattice without resistance below the superconducting transition temperature $T_c$. Electron Cooper pairs in most superconductors form anti-parallel spin singlets with total spin S = 0, although they can also form parallel spin-triplet Cooper pairs with S = 1 and an odd parity wavefunction. Spin-triplet pairing is important because it can host topological states and Majorana fermions relevant for quantum computation. Because spin-triplet pairing is usually mediated by ferromagnetic (FM) spin fluctuations3, uranium-based materials near an FM instability are considered to be ideal candidates for realizing spin-triplet superconductivity. Indeed, UTe 2 , which has a $T_c$ ≈ 1.6 K, has been identified as a candidate for a chiral spin-triplet topological superconductor near an FM instability, although it also has antiferromagnetic (AF) spin fluctuations. Here we use inelastic neutron scattering (INS) to show that superconductivity in UTe 2 is coupled to a sharp magnetic excitation, termed resonance, at the Brillouin zone boundary near AF order. Because the resonance has only been found in spin-singlet unconventional superconductors near an AF instability, its observation in UTe 2 suggests that AF spin fluctuations may also induce spin-triplet pairing or that electron pairing in UTe 2 has a spin-singlet component.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2026

Non-Altermagnetic Origin of Exchange Bias Behaviors in Incoherent RuO 2 /Fe Bilayer Heterostructures

Initially identified as a promising altermagnetic (AM) candidate, rutile RuO 2 has since become embroiled in controversy due to contradictory findings of modeling and measurements of the magnetic properties of bulk crystals and thin films. For example, despite observations of a bulk nonmagnetic state using density functional theory, neutron scattering, and muon spin resonance measurements, patterned RuO 2 Hall bars and film heterostructures display magnetotransport signatures of magnetic ordering. Among the characteristics routinely cited as evidence for AM is the observation of exchange bias (EB) in an intimately contacted Fe-based ferromagnetic (FM) layer, which can arise due to interfacial coupling with a compensated antiferromagnet. Here, within this work, the origins of this EB coupling in Ru-capped RuO 2 /Fe bilayers are investigated using polarized neutron diffraction, polarized neutron reflectometry, cross-sectional transmission electron microscopy, and super conducting quantum interference device measurements. These experiments reveal that the EB behavior is driven by the formation of an iron oxide interlayer containing Fe 3 O 4 that undergoes a magnetic transition and pins interfacial moments within Fe at low temperature. These findings are confirmed by comparable measurements of Ni-based heterostructures, which do not display EB coupling, as well as magnetometry of additional Fe/Ru bilayers that display oxide-driven EB coupling despite the absence of the epitaxial RuO 2 layer. While these results do not directly refute the possibility of AM ordering in RuO 2 thin films, they reveal that EB, and related magnetotransport phenomena, cannot alone be considered evidence of this characteristic in the rutile structure due to interfacial chemical disorder.

RuO2↗
DOE OSTI2014

Quantum pumping of valley current in strain engineered graphene

We studied the generation of valley dependent current by adiabatic quantum pumping in monolayer graphene in the presence of electric potential barriers, ferromagnetic field and strain. The pumped currents in the two valleys have same magnitudes and opposite directions; thus, a pure valley current is generated. The oscillation of the pumped pure valley current is determined by the Fabry-Perot resonances formed in the structure. In our calculation, the pumped pure valley current can be as high as 50 nA, which is measurable using present technologies. The proposed device is useful for the development of graphene valleytronic devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Element-resolved thermodynamics of magnetocaloric LaFe 13 – x Si x

By combination of two independent approaches, nuclear resonant inelastic x-ray scattering and first-principles calculations in the framework of density functional theory, we demonstrate significant changes in the element-resolved vibrational density of states across the first-order transition from the ferromagnetic low temperature to the paramagnetic high temperature phase of LaFe 13-x Si x . These changes originate from the itinerant electron metamagnetism associated with Fe and lead to a pronounced magneto-elastic softening despite the large volume decrease at the transition. As a result, the increase in lattice entropy associated with the Fe subsystem is significant and contributes cooperatively with the magnetic and electronic entropy changes to the excellent magneto- and barocaloric properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Relationship between A-site cation and magnetic structure in 3d–5d–4f double perovskite iridates Ln 2 NiIrO 6 ( Ln = La, Pr, Nd)

We report a comprehensive investigation of Ln 2 NiIrO 6 (Ln=La, Pr, Nd) using thermodynamic and transport properties, neutron powder diffraction, resonant inelastic x-ray scattering, and density-functional theory (DFT) calculations to investigate the role of A-site cations on the magnetic interactions in this family of hybrid 3d–5d–4f compositions. Magnetic structure determination using neutron diffraction reveals antiferromagnetism for La 2 NiIrO 6 , a collinear ferrimagnetic Ni and Ir state that is driven to long-range antiferromagnetism upon the onset of Nd ordering in Nd 2 NiIrO 6 , and a noncollinear ferrimagnetic Ni and Ir sublattice interpenetrated by a ferromagnetic Pr lattice for Pr 2 NiIrO 6 . For Pr 2 NiIrO 6 , heat-capacity results reveal the presence of two independent magnetic sublattices, and transport resistivity indicates insulating behavior and a conduction pathway that is thermally mediated. Here, a first principles DFT calculation elucidates the existence of the two independent magnetic sublattices within Pr 2 NiIrO 6 and offers insight into the behavior in La 2 NiIrO 6 and Nd 2 NiIrO 6 . Resonant inelastic x-ray scattering is consistent with spin-orbit coupling splitting the t 2 g manifold of octahedral Ir 4+ into a J eff = 1/2 and J eff = 3/2 state for all members of the series considered.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Spin dependent resonant electron tunneling through planar graphene barriers

Here, we study spin-dependent electron transport properties of two dimensional graphene double and triple barrier junctions via first-principles calculations. The double barrier junction consists of two graphene leads, a quantum well of zigzag graphene nanoribbon (ZGNR) in the center, and two vacuum barriers separating the ZGNR from the two leads. Resonant electron tunneling occurs when the energy bands of graphene and ZGNR are well aligned in energy and wavevector. Highly spin-polarized electron transmission arises in such junctions when the two edges of the center ZGNR are in the ferromagnetic configuration. The spin polarization of the electron transmission at the Fermi energy can be tuned by gate voltage. We further investigate the dependence of the electron transmission on the width of the ZGNR, effects on barrier height when replacing vacuum by h-BN, and the consequence of replacing a double barrier by a triple barrier.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Asymmetric magnetic proximity effect in a Pd/Co/Pd trilayer system

In spintronic devices consisting of ferromagnetic/nonmagnetic systems, the ferromagnet-induced magnetic moment in the adjacent nonmagnetic material significantly influences the spin transport properties. In this study, such magnetic proximity effect in a Pd/Co/Pd trilayer system is investigated by x-ray magnetic circular dichroism and x-ray resonant magnetic reflectivity, which enables magnetic characterizations with element and depth resolution. We observe that the total Pd magnetic moments induced at the top Co/Pd interface are significantly larger than the Pd moments at the bottom Pd/Co interface, whereas transmission electron microscopy and reflectivity analysis indicate the two interfaces are nearly identical structurally. Furthermore, such asymmetry in magnetic proximity effects could be important for understanding spin transport characteristics in ferromagnetic/nonmagnetic systems and its potential application to spin devices.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Magnetic structure of Nd in NdFeAsO studied by x-ray resonant magnetic scattering

The magnetic structure of Nd in NdFeAsO compound has been explored by x-ray resonant magnetic scattering at the Nd L 2 edge ( E = 6.725 keV) at 1.7 ≤ T ≤ 15 K. At T = 1.7 K we find that the Nd moments are aligned along the crystallographic c direction with the (1, 0, 0) propagation vector, and are arranged antiferromagnetically along the a direction and ferromagnetically along the b and c directions. At 1.7 < T ≤ 15 K, we observe an unusual temperature dependence of the magnetic Bragg peaks that appear differently at Q = ( h , 0 , l ) and ( 0 , k , l ) . From the changes of magnetic intensities and our representation analysis, we find that the Nd moments are reoriented toward the a direction with a gradual decrease of the moment component in the c direction with increasing temperature. We postulate that the reorientation of the Nd moment is due to a strong interplay with the Fe moment which is fully ordered in this temperature range.

36 MATERIALS SCIENCE↗
DOE OSTI2013

CoxC nanorod magnets: Highly magnetocrystalline anisotropy with lower Curie temperature for potential applications

Magnetic CoxC nanorods with larger magnetocrystalline anisotropy of 5 x 10(5) J/m(3) as well as larger coercivity and lower Curie temperature are introduced. The particles have an average diameter of 8 nm and shows three different magnetic behaviors. The sample shows ferromagnetism up to 400 K, superparamagnetism at temperature > 400 K and <T-C (465 K) and paramagnetism above 465 K. Such different behaviors open the door for various applications such as permanent magnets, magnetic sensors and contract agent for magnetic resonance imaging. (c) 2013 Elsevier B.V. All rights reserved.

El-Gendy, AA↗
DOE OSTI2014

Anomalous temperature dependence in valence band spectra: A resonant photoemission study of layered perovskite Sr{sub 2}CoO{sub 4}

Valence band spectra (VBS) and its modification across Curie temperature (T{sub C}) of Sr{sub 2}CoO{sub 4} thin film are studied using resonant photoemission spectroscopy. It is found that VBS mainly consists of hybridized states of Co-3d t{sub 2g}e{sub g} and O-2p; however, Co-3d e{sub g} states show its prominence only in the ferromagnetic temperature regime. Below T{sub C}, spectral weight transfer takes place anomalously from high binding energy (B.E.) region to low B.E. region, signifying the enhanced intermediate or low spin state Co{sup 4+} ions. It is suggested that spin-lattice coupling and many-body effects in Sr{sub 2}CoO{sub 4} derived from the strong electron correlations lead to such temperature dependence of VBS.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗