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At least 1,243 records · Page 69
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Robust Quantum Hall Ferromagnetism near a Gate-Tuned ν = 1 Landau Level Crossing

In a low-disorder two-dimensional electron system, when two Landau levels of opposite spin or pseudospin cross at the Fermi level, the dominance of the exchange energy can lead to a ferromagnetic, quantum Hall ground state whose gap is determined by the exchange energy and has skyrmions as its excitations. This is normally achieved via applying either hydrostatic pressure or uniaxial strain. Here, we study here a very high-quality, low-density, two-dimensional hole system, confined to a 30-nm-wide (001) GaAs quantum well, in which the two lowest-energy Landau levels can be gate tuned to cross at and near filling factor v = 1. As we tune the field position of the crossing from one side of v = 1 to the other by changing the hole density, the energy gap for the quantum Hall state at v =1 remains exceptionally large, and only shows a small dip near the crossing. The gap overall follows a $\sqrt{B}$ dependence, expected for the exchange energy. Our data are consistent with a robust quantum Hall ferromagnet as the ground state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Screening of Polar Electron-Phonon Interactions near the Surface of the Rashba Semiconductor BiTeCl

Understanding electron-phonon coupling in noncentrosymmetric materials is critical for controlling the internal fields which give rise to Rashba interactions. We apply time- and angle-resolved photoemission spectroscopy (trARPES) to study coherent phonons in the surface and bulk regions of the polar semiconductor BiTeCl. Aided by \textit{ab initio} calculations, our measurements reveal the coupling of out-of-plane $A_1$ modes and an in-plane $E_2$ mode. By considering how these modes modulate the electric dipole moment in each unit cell, we show that the polar $A_1$ modes are more effectively screened in the metallic surface region, while the non-polar $E_2$ mode couples in both regions. Finally, in addition to informing strategies to optically manipulate Rashba interactions, this work has broader implications for the behavior of electron-phonon coupling in systems characterized by inhomogeneous dielectric environments.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Topological Defect Mediated Helical Phase Reorientation by Uniaxial Stress

Strain engineering enables precise, energy-efficient control of nanoscale magnetism. However, unlike well-studied strain-dislocation interactions in mechanical deformation, the spatial evolution of strain-induced spin rearrangement remains poorly understood. Using Lorentz transmission electron microscopy, we manipulate and observe helical domain reorientation under quantitatively applied uniaxial tensile stress. Our findings reveal striking similarity to plastic deformation in metals, where the critical stress for propagation vector ( Q ) reorientation depends on its angle with the stress direction. Magnetic defects mediate reorientation via “break-and-reconnect” or “dislocation gliding–annihilation” processes. Simulations confirm that strain-induced anisotropic Dzyaloshinskii-Moriya interaction may play a key role. These insights advance strain-driven magnetism and offer a promising route for energy-efficient magnetic nanophase control in next-generation information technology. Published by the American Physical Society 2025

36 MATERIALS SCIENCE↗
DOE OSTI2022

Partial densities of states from x-ray absorption and Auger electron spectroscopy: Use of core-hole memory

Ag L 3 edge x-ray absorption and L 3 −M 4,5 M 4,5 Auger electron spectra have been measured and simulated for a variety of x-ray electric-field polarization and Auger electron emission directions. The theory relies on density-functional theory, use of the Bethe–Salpeter equation, atomic multiplet theory, and a simplified model for the Auger line shape and its dependence on photon energy. We also demonstrate that partial densities of states for dT 2g , dE g , and sA g symmetry partial-wave channels at the Ag site in the solid can be deduced from the experimental measurements with only atomic theoretical input, i.e., with no solid-state theory other than assuming a Fermi edge.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Searching for synchrotron emission from the geminga TeV halo using the planck satellite

Pulsars convert a significant fraction of their total spin-down power into very high-energy electrons, leading to the formation of TeV halos. While these halos are well characterized at TeV energies, it remains unclear whether pulsars also accelerate electrons efficiently at lower energies and how these particles propagate through their surrounding environments. We aim to test whether synchrotron emission from $\sim 50$–$300 \, \textrm{GeV}$ electrons around the Geminga pulsar can be detected in the frequency range observed by the Planck satellite. This would help constrain low-energy particle acceleration and diffusion in the vicinity of pulsars. We model the expected synchrotron emission from Geminga’s TeV halo based on various diffusion and injection spectrum scenarios and compare these predictions to publicly available multi-frequency Planck data. We find no conclusive evidence of spatially extended synchrotron emission associated with Geminga in any of Planck’s frequency bands. Our calculations show that even under favorable diffusion and injection conditions, the predicted synchrotron flux lies well below Planck’s measured background levels.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Low-temperature MnBi alloys: Electronic and magnetic properties, constitution, morphology and fabrication (Review article)

The article reviews the rich phenomena of physical properties of MnBi. The diverse phenomena include strong spin-orbit interaction, anomalous temperature dependence of the coercivity and the magneto-crystalline anisotropy field, unique magneto-optical properties. Issues addressed include the nature of the electronic ground states of MnBi, the electronic and magnetic structures, Fermi surface, magneto-crystalline anisotropy, x-ray magnetic dichroism. The discussion includes key experiments, such as optical and magneto-optical spectroscopic measurements, de Haas-van Alphen (dHvA) measurements, x-ray photoemission and x-ray absorption spectroscopy measurements as well as x-ray magnetic circular dichroism. The effect of the spin-orbit (SO) interaction and Coulomb repulsion U were found to be crucial for the Fermi surface, cyclotron masses, magneto-optical properties, and x-ray magnetic circular dichroism. The microscopic origin of unique magneto-crystalline anisotropy and giant Kerr effect in MnBi is analyzed in detail. The huge Kerr effect in MnBi is caused by the combination of a sizable magnetic moment on manganese, the large spin-orbit coupling of bismuth, and a strong hybridization between the manganese 3d and the bismuth 6p states. The magneto-optically active states are mainly the 6p states of Bi. We show that the observed temperature dependence of the magneto-crystalline anisotropy can be explained taking into account the spin-orbit interaction together with strong Coulomb electron-electron interaction. The SO coupling of Bi is equally responsible for the large magneto-crystalline anisotropy energy as is the exchange splitting of Mn. The fabrication, morphology, and constitution of low-temperature MnBi alloys in bulk, thin films, and nanoparticles are discussed. The nanocomposite permanent magnetic materials based on MnBi, (Co, Fe) and Nd 2 Fe 14 B are also discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Controlled Single-Electron Transfer via Metal–Ligand Cooperativity Drives Divergent Nickel-Electrocatalyzed Radical Pathways

Electrocatalysis enables the construction of C-C bonds under mild conditions via controlled formation of carbon-centered radicals. For sequences initiated by alkyl halide reduction, coordinatively unsaturated Ni complexes commonly serve as single-electron transfer agents, giving rise to the foundational question of whether outer- or inner-sphere electron transfer oxidative addition prevails in redox mediation. Indeed, rational design of electrochemical processes requires the discrimination of these two electron transfer pathways, as they can have outsized effects on the rate of substrate bond activation and thus impact radical generation rates and downstream product selectivities. We present results from combined synthetic, electroanalytical, and computational studies that examine the mechanistic differences of single electron transfer to alkyl halides imparted by Ni metal-ligand cooperativity. Electrogenerated reduced Ni species, stabilized by delocalized spin density onto a redox-active tpyPY2Me polypyridyl ligand, activates alkyl iodides via outer-sphere electron transfer, allowing for the selective activation of alkyl iodide substrates over halogen atom donors and the controlled generation and sequestration of electrogenerated radicals. In contrast, the Ni complex possessing a redox-innocent pentapyridine congener activates the substrates in an inner-sphere fashion owning to a purely metal-localized spin, thereby activating both substrates and halogen atom donors in an indiscriminate fashion, generating a high concentration of radicals and leading to unproductive dimerization. Overall, our data establish that controlled electron transfer via Ni-ligand cooperativity can be used to limit undesired radical recombination products and promote selective radical processes in electrochemical environments, providing a generalizable framework for designing redox mediators with distinct rate and potential requirements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Spin density wave and van Hove singularity in the kagome metal CeTi 3 Bi 4

Kagome metals with van Hove singularities near the Fermi level can host intriguing quantum phenomena such as chiral loop currents, electronic nematicity, and unconventional superconductivity. However, to our best knowledge, unconventional magnetic states driven by van Hove singularities–like spin-density waves–have not been observed experimentally in kagome metals. Here, we report the magnetic and electronic structure of the layered kagome metal CeTi 3 Bi 4 , where Ti kagome electronic structure interacts with a magnetic sublattice of Ce 3+ J eff = 1/2 moments. Neutron diffraction reveals an incommensurate spin-density wave ground state of the Ce 3+ moments, coexisting with commensurate antiferromagnetic order across most of the temperature-field phase diagram. The commensurate component is preferentially suppressed by thermal fluctuations and magnetic field, yielding a rich phase diagram involving an intermediate single-Q spin-density wave phase. First-principles calculations and angle-resolved photoemission spectroscopy identify van Hove singularities near the Fermi level, with the observed magnetic propagation vectors connecting their high density of states, strongly suggesting a van Hove singularity-assisted spin-density wave. These findings establish kagome metals LnTi 3 Bi 4 as a model platform where the characteristic electronic structure of the kagome lattice plays a pivotal role in magnetic order.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Electronic Structures of Iron in Oxide Glasses via 1s3p Resonant Inelastic X-ray Scattering

Electronic structures of iron in glasses are essential for unraveling the effect of transition metals on amorphous networks and controlling the electro-optical and transport properties of advanced glasses and amorphous energy-storing materials. The electronic configurations around iron in glasses, however, remain not well understood due to the structural disorders arising from multiple iron species with distinct valence, coordination, and spin states. Here, the first 1s3p resonant inelastic X-ray scattering (RIXS) for oxide glasses identifies hidden electronic configurations for Fe 2+ and Fe 3+ in amorphous networks. The results allow us to quantify the composition-induced evolution of oxygen ligand–field interactions of high-spin Fe 3d states with varying valence and coordination environments in complex glasses. The distinct electronic structures account for the electronic origins of iron-induced changes in the glass properties. The results offer prospects for a simultaneous probing of valence, coordination, and spin states of transition metals in diverse multicomponent oxide glasses and functional amorphous solids via 1s3p RIXS.

Kim, Yong-Hyun [Seoul National Univ. (Korea, Repub↗
DOE OSTI2020

Curved Three-Dimensional Cobalt Nanohelices for Use in Domain Wall Device Applications

Three-dimensional fabrication of nanostructures opens new possibilities to not only understand the fundamental effects of shape and of the interactions between the nanostructures, but also to develop novel technological applications. Of course, this is of particular importance for magnetic nanostructures, where curvilinear geometry can lead to the emergence of novel topological effects and spin excitations. In this work, we have used the focused electron beam ion deposition (FEBID) method to fabricate three-dimensional magnetic cobalt nanohelices with controlled geometry such as chirality, and curvature. Additionally, using a combination of off-axis electron holography and electron tomography, we are able to determine the way in which the quantitative nanoscale magnetization distribution is related to the 3D morphology and curvature of the nanohelices. These results pave a way forward for development of future 3D magnetic nanostructures to explore novel physics as well as for applications such as magnetic field sensors, spin-wave filters, and magneto-optical devices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Direct light–induced spin transfer between different elements in a spintronic Heusler material via femtosecond laser excitation

Heusler compounds are exciting materials for future spintronics applications because they display a wide range of tunable electronic and magnetic interactions. Here, we use a femtosecond laser to directly transfer spin polarization from one element to another in a half-metallic Heusler material, Co 2 MnGe. This spin transfer initiates as soon as light is incident on the material, demonstrating spatial transfer of angular momentum between neighboring atomic sites on time scales < 10 fs. Using ultrafast high harmonic pulses to simultaneously and independently probe the magnetic state of two elements during laser excitation, we find that the magnetization of Co is enhanced, while that of Mn rapidly quenches. Density functional theory calculations show that the optical excitation directly transfers spin from one magnetic sublattice to another through preferred spin-polarized excitation pathways. This direct manipulation of spins via light provides a path toward spintronic devices that can operate on few-femtosecond or faster time scales.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Harmonic generation predominantly from a single spin channel in a half metal

Harmonic generation in atoms and molecules has reshaped our understanding of ultrafast phenomena beyond the traditional nonlinear optics and has launched attosecond physics. Harmonics from solids represent a new frontier, where both majority and minority spin channels contribute to harmonics. This is true even in a ferromagnet whose electronic states are equally available to optical excitation. In this work, we demonstrate that harmonics can be generated {mostly} from a single spin channel in half metallic chromium dioxide. An energy gap in the minority channel greatly reduces the harmonic generation, so harmonics predominantly emit from the majority channel, with a small contribution from the minority channel. However, this is only possible when the incident photon energy is well below the energy gap in the minority channel, so all the transitions in the minority channel are virtual. The onset of the photon energy is determined by the transition energy between the dipole-allowed transition between the O-$2p$ and Cr-$3d$ states. Harmonics mainly from a single spin channel can be detected, regardless of laser field strength, as far as the photon energy is below the minority band energy gap. This prediction should be tested experimentally

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Advances and Challenges of SCAN and r 2 SCAN Density Functionals in Transition‐Metal Compounds

ABSTRACT Transition‐metal compounds (TMCs) with open‐shell d ‐electrons are characterized by a complex interplay of lattice, charge, orbital, and spin degrees of freedom, giving rise to various fascinating applications. Often exhibiting exotic properties, these compounds are commonly classified as correlated systems due to strong inter‐electronic interactions called Hubbard U . This inherent complexity presents significant challenges to Kohn‐Sham density functional theory (KS‐DFT), the most widely used electronic structure method in condensed matter physics and materials science. While KS‐DFT is, in principle, exact for the ground‐state total energy, its exchange‐correlation energy must be approximated in practice. The mean‐field nature of KS implementations, combined with the limitations of current exchange‐correlation density functional approximations, has led to the perception that DFT is inadequate for correlated systems, particularly TMCs. Consequently, a common workaround involves augmenting DFT with an on‐site Hubbard‐like U correction. In recent years, the strongly constrained and appropriately normed (SCAN) density functional, along with its refined variant r 2 SCAN, has achieved remarkable progress in accurately describing the structural, energetic, electronic, magnetic, and vibrational properties of TMCs, challenging the traditional perception of DFT's limitations. This review explores the design principles of SCAN and r 2 SCAN, highlights their key advancements in studying TMCs, explains the mechanisms driving these improvements, and addresses the remaining challenges in this evolving field.

Zhang, Yubo [Minjiang Collaborative Center for The↗
DOE OSTI2024

Growth and characterization of ferromagnetic Ga 2 O 3 :(Cr, Mn)

The goal of this Exploratory Express project was to explore the possibility of tunable ferromagnetism in Mn or Cr incorporated epitaxial Ga 2 O 3 films. Tunability of magnetic properties can enable novel applications in spintronics, quantum computing, and magnetism-based logics by allowing control of magnetism down to the nanoscale. Carriers (electrons or holes) mediated ferromagnetic ordering in semiconductor can lead to tunable ferromagnetism by leveraging the tunability of carrier density with doping level, gate electric field, or optical pumping of the carriers. The magnetic ions (Cr or Mn) in Ga 2 O 3 act as localized spin centers which can potentially be magnetically coupled through conduction electrons to enable ferromagnetic ordering. Here we investigated tunable ferromagnetism in beta Ga 2 O 3 semiconductor host with various n-doping levels by incorporating 2.4 atomic percent Mn or Cr. The R&D approach involved growth of epitaxial Ga 2 O 3 film on sapphire or Ga 2 O 3 substrate, implantation of Mn or Cr ions, annealing of the samples post implantation, and magnetic measurements. We studied magnetic behavior of Mn:Ga 2 O 3 as a function of different n-doping levels and various annealing temperatures. The vibrating sample magnetometry (VSM) measurement exhibited strong ferromagnetic signals from the annealed Mn:Ga 2 O 3 sample with n-doping level of 5E19 cm -3 . This ferromagnetic behavior disappears from Mn:Ga 2 O 3 when the n-doping level is reduced to 5E16 cm -3 . Although these results are to be further verified by other measurement schemes due to the observation of background ferromagnetism from the growth substrate, these results indicate the possibility of tunable ferromagnetism in Mn:Ga 2 O 3 mediated by conduction electrons.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Electronic and magnetic properties of quasi-one-dimensional osmium halide OsCl 4

Using ab initio density functional theory, we study the electronic and magnetic properties of the van der Waals chain material OsCl 4 . In the nonmagnetic state, a strongly anisotropic band structure was observed, in agreement with its anticipated one-dimensional crystal geometry. Based on Wannier functions, we found that the four electrons of the 5d Os atom form a low-spin S = 1 state, with a large crystal field between the d xz/yz and d xy orbitals, corresponding to a strong Jahn–Teller distortion (Q 3 < 0). As a consequence, the magnetic properties are mainly contributed by the d xz/yz states. Furthermore, when a Mott gap develops after the introduction of the Hubbard U and Hund coupling J, we found that the staggered spin order is the most likely magnetic state, namely, spins arranged as (↑-↓-↑-↓) with π wavevector along the chain. In addition, the energy differences between various spin states are small, suggesting a weak magnetic exchange coupling along the chain. Overall, our results provide guidance to experimentalists and theorists working on quasi-one-dimensional osmium halides chain materials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Chemical Design of Spin Frustration to Realize Topological Spin Glasses

Patterning spins to generate collective behavior is at the core of condensed matter physics. Physicists develop techniques, including the fabrication of magnetic nanostructures and precision layering of materials specifically to engender frustrated lattices. As chemists, we can access such exotic materials through targeted chemical synthesis and create new lattice types by chemical design. Here, in this study, we introduce a new approach to induce magnetic frustration on a modified honeycomb lattice through a competition of alternating antiferromagnetic (AFM) and ferromagnetic (FM) nearest-neighbor interactions. By subtly modulating these two types of interactions through facile synthetic modifications, we created two systems: (1) a topological spin glass and (2) a frustrated spin-canted magnet with low-temperature exchange bias. To design this unconventional magnetic lattice, we used a metal–organic framework (MOF) platform, Ni 3 (pymca) 3 X 3 (NipymcaX where pymca = pyrimidine-2-carboxylato and X = Cl, Br). We isolated two MOFs, NipymcaCl and NipymcaBr, featuring canted Ni 2+ -based moments. Despite this similarity, differences in the single-ion anisotropies of the Ni 2+ spins result in distinct magnetic properties for each material. NipymcaCl is a topological spin glass, while NipymcaBr is a rare frustrated magnet with low-temperature exchange bias. Density functional theory calculations and Monte Carlo simulations on the NipymcaX lattice support the presence of magnetic frustration as a result of alternating AFM and FM interactions. Our calculations enabled us to determine the ground-state spin configuration and the distribution of spin–spin correlations relative to paradigmatic kagomé and triangular lattices. This modified honeycomb lattice is similar to the electronic Kekulé-O phase in graphene and provides a highly tunable platform to realize unconventional spin physics.

Exchange bias↗
DOE OSTI2024

Development of (NO)Fe(N 2 S 2 ) as a Metallodithiolate Spin Probe Ligand: A Case Study Approach

The ubiquity of sulfur–metal connections in nature inspires the design of bi- and multimetallic systems in synthetic inorganic chemistry. Common motifs for biocatalysts developed in evolutionary biology include the placement of metals in close proximity with flexible sulfur bridges as well as the presence of π-acidic/delocalizing ligands. This Account will delve into the development of a (NO)Fe(N 2 S 2 ) metallodithiolate ligand that harnesses these principles. The Fe(NO) unit is the centroid of a N 2 S 2 donor field, which as a whole is capable of serving as a redox-active, bidentate S-donor ligand. Its paramagnetism as well as the ν(NO) vibrational monitor can be exploited in the development of new classes of heterobimetallic complexes. We offer four examples in which the unpaired electron on the {Fe(NO)} 7 unit is spin-paired with adjacent paramagnets in proximal and distal positions. First, the exceptional stability of the (NO)Fe(N 2 S 2 )-Fe(NO) 2 platform, which permits its isolation and structural characterization at three distinct redox levels, is linked to the charge delocalization occurring on both the Fe(NO) and the Fe(NO) 2 supports. This accommodates the formation of a rare nonheme {Fe(NO)} 8 triplet state, with a linear configuration. A subsequent FeNi complex, featuring redox-active ligands on both metals (NO on iron and dithiolene on nickel), displayed unexpected physical properties. Our research showed good reversibility in two redox processes, allowing isolation in reduced and oxidized forms. Various spectroscopic and crystallographic analyses confirmed these states, and Mössbauer data supported the redox change at the iron site upon reduction. Oxidation of the complex produced a dimeric dication, revealing an intriguing magnetic behavior. The monomer appears as a spin-coupled diradical between {Fe(NO)} 7 and the nickel dithiolene monoradical, while dimerization couples the latter radical units via a Ni 2 S 2 rhomb. Magnetic data (SQUID) on the dimer dication found a singlet ground state with a thermally accessible triplet state that is responsible for magnetism. A theoretical model built on an H 4 chain explains this unexpected ferromagnetic low-energy triplet state arising from the antiferromagnetic coupling of a four-radical molecular conglomerate. For comparison, two (NO)Fe(N 2 S 2 ) were connected through diamagnetic group 10 cations producing diradical trimetallic complexes. Antiferromagnetic coupling is observed between {Fe(NO)} 7 units, with exchange coupling constants (J) of -3, -23, and -124 cm –1 for Ni II , Pd II , and Pt II , respectively. This trend is explained by the enhanced covalency and polarizability of sulfur-dense metallodithiolate ligands. A central paramagnetic trans-Cr(NO)(MeCN) receiver unit core results in a cissoid structural topology, influenced by the stereoactivity of the lone pair(s) on the sulfur donors. This {Cr(NO)} 5 radical bridge, unlike all previous cases, finds the coupling between the distal Fe(NO) radicals to be ferromagnetic (J = 24 cm –1 ). The stability and predictability of this S = 1/2 moiety and the steric/electronic properties of the bridging thiolate sulfurs suggest it to be a likely candidate for the development of novel molecular (magnetic) compounds and possibly materials. The role of synthetic inorganic chemistry in designing synthons that permit connections of the (NO)Fe(N 2 S 2 ) metalloligand is highlighted as well as the properties of the heterobi- and polymetallic complexes derived therefrom.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Liquid-like spin dynamics in a hybrid Heisenberg-Ising antiferromagnet

Two-dimensional (2D) materials and their heterostructures enable unconventional electronic properties and functionalities not accessible in their bulk counterparts. This approach is now being extended to magnetic materials to engineer their spin structures and magnetic fields produced by them. However, spin dynamics of 2D magnetic heterostructures remain largely unexplored. Here, we demonstrate that heterointerfacing Heisenberg square-lattice antiferromagnet (AF) Sr 2 IrO 4 with its bilayer variant Ising AF Sr 3 Ir 2 O 7 in a superlattice leads to liquid-like spin dynamics in the former, characterized by slow recovery of the AF order after its transient suppression by an optical pump, and complete absence of spin waves except in an immediate vicinity of the ordering wavevector. Instead, the spin excitation spectra are dominated by isotropic continua, which in previous works have been interpreted as fractional spin excitations, or spinons, that extends to unprecedentedly low energies. Thus, our results provide a pathway to frustrated magnetism in square lattices by heterointerfacing two distinct types of AFs.

RIXS↗