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At least 685 records · Page 38

All sources NASA NTRS DOE OSTI

DOE OSTI2018

Discovery of coexisting Dirac and triply degenerate magnons in a three-dimensional antiferromagnet

Topological magnons are emergent quantum spin excitations featured by magnon bands crossing linearly at the points dubbed nodes, analogous to fermions in topological electronic systems. Experimental realisation of topological magnons in three dimensions has not been reported so far. Here, by measuring spin excitations (magnons) of a three-dimensional antiferromagnet Cu3TeO6 with inelastic neutron scattering, we provide direct spectroscopic evidence for the coexistence of symmetry-protected Dirac and triply degenerate nodes, the latter involving three-component magnons beyond the Dirac–Weyl framework. Our theoretical calculations show that the observed topological magnon band structure can be well described by the linear-spin-wave theory based on a Hamiltonian dominated by the nearest neighbour exchange interaction J1. As such, we showcase Cu3TeO6 as an example system where Dirac and triply degenerate magnonic nodal excitations coexist, demonstrate an exotic topological state of matter, and provide a fresh ground to explore the topological properties in quantum materials.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Dynamic fingerprint of fractionalized excitations in single-crystalline Cu3Zn(OH)6FBr

Abstract Beyond the absence of long-range magnetic orders, the most prominent feature of the elusive quantum spin liquid (QSL) state is the existence of fractionalized spin excitations, i.e., spinons. When the system orders, the spin-wave excitation appears as the bound state of the spinon-antispinon pair. Although scarcely reported, a direct comparison between similar compounds illustrates the evolution from spinon to magnon. Here, we perform the Raman scattering on single crystals of two quantum kagome antiferromagnets, of which one is the kagome QSL candidate Cu 3 Zn(OH) 6 FBr, and another is an antiferromagnetically ordered compound EuCu 3 (OH) 6 Cl 3 . In Cu 3 Zn(OH) 6 FBr, we identify a unique one spinon-antispinon pair component in the E 2g magnetic Raman continuum, providing strong evidence for deconfined spinon excitations. In contrast, a sharp magnon peak emerges from the one-pair spinon continuum in the E g magnetic Raman response once EuCu 3 (OH) 6 Cl 3 undergoes the antiferromagnetic order transition. From the comparative Raman studies, we can regard the magnon mode as the spinon-antispinon bound state, and the spinon confinement drives the magnetic ordering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Decay and renormalization of a longitudinal mode in a quasi-two-dimensional antiferromagnet

Abstract An ongoing challenge in the study of quantum materials, is to reveal and explain collective quantum effects in spin systems where interactions between different modes types are important. Here we approach this problem through a combined experimental and theoretical study of interacting transverse and longitudinal modes in an easy-plane quantum magnet near a continuous quantum phase transition. Our inelastic neutron scattering measurements of Ba 2 FeSi 2 O 7 reveal the emergence, decay, and renormalization of a longitudinal mode throughout the Brillouin zone. The decay of the longitudinal mode is particularly pronounced at the zone center. To account for the many-body effects of the interacting low-energy modes in anisotropic magnets, we generalize the standard spin-wave theory. The measured mode decay and renormalization is reproduced by including all one-loop corrections. The theoretical framework developed here is broadly applicable to quantum magnets with more than one type of low energy mode.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Hybrid spin Hall nano-oscillators based on ferromagnetic metal/ferrimagnetic insulator heterostructures

Abstract Spin-Hall nano-oscillators (SHNOs) are promising spintronic devices to realize current controlled GHz frequency signals in nanoscale devices for neuromorphic computing and creating Ising systems. However, traditional SHNOs devices based on transition metals have high auto-oscillation threshold currents as well as low quality factors and output powers. Here we demonstrate a new type of hybrid SHNO based on a permalloy (Py) ferromagnetic-metal nanowire and low-damping ferrimagnetic insulator, in the form of epitaxial lithium aluminum ferrite (LAFO) thin films. The superior characteristics of such SHNOs are associated with the excitation of larger spin-precession angles and volumes. We further find that the presence of the ferrimagnetic insulator enhances the auto-oscillation amplitude of spin-wave edge modes, consistent with our micromagnetic modeling. This hybrid SHNO expands spintronic applications, including providing new means of coupling multiple SHNOs for neuromorphic computing and advancing magnonics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Systematic determination of a material’s magnetic ground state from first principles

Abstract We present a self-consistent method based on first-principles calculations to determine the magnetic ground state of materials, regardless of their dimensionality. Our methodology is founded on satisfying the stability conditions derived from the linear spin wave theory (LSWT) by optimizing the magnetic structure iteratively. We demonstrate the effectiveness of our method by successfully predicting the experimental magnetic structures of NiO, FePS 3 , FeP, MnF 2 , FeCl 2 , and CuO. In each case, we compared our results with available experimental data and existing theoretical calculations reported in the literature. Finally, we discuss the validity of the method and the possible extensions.

Chemistry↗

DOE OSTI2025

A magnon band analysis of GdRu 2 Si 2 in the field-polarized state

Understanding the formation of skyrmions in centrosymmetric materials is a problem of fundamental and technological interest. GdRu 2 Si 2 is a candidate material that hosts a variety of multi-Q magnetic phases, including in zero-field. Here, inelastic neutron scattering is used to measure the spin excitations in the field-polarized phase of GdRu 2 Si 2 . Linear spin wave theory and a method of interaction invariant path analysis are used to derive a Hamiltonian accounting for the spectra. The Hamiltonian, dominated by bilinear (Ruderman-Kittel-Kasuya-Yosida) Heisenberg exchange, compares favorably to ab initio calculations. Dipolar interactions are a secondary energy scale to consider, with J D.D ~ 0.05 J RKKY . However, it is shown that in the field-polarized phase the dipolar interactions ‘self screen’ so that their effect is largely suppressed. No specific evidence for higher-order exchange is found. These aspects are discussed in the context of the lower field multi-Q states and the anisotropy of the system.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Operando microscopy for neuromorphic hardware

Microscopy techniques can uncover the physical properties and dynamic behaviours of materials, driving the discovery of emergent phenomena and guiding the design of next-generation computing hardware. As artificial intelligence becomes pervasive, the demand for high-performance materials to support sustainable information technologies is growing. Here, this Review highlights state-of-the-art imaging from electron and X-ray to optical techniques to probe the dynamics of neuromorphic materials, including operando characterization of devices. We examine design principles for neuromorphic materials, along with obstacles that hinder their development. Emphasis is placed on spatially and temporally resolved approaches that capture state changes including phase transitions, ferroic switching and spin-wave propagation that emulate biological components such as neurons, synapses and their connectivity. We discuss challenges in operando characterization and the integration of artificial intelligence-driven analysis for feedback-guided material discovery. Finally, we outline opportunities for real-time imaging of neuromorphic systems, paving the way towards adaptive, brain-inspired hardware.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Hybridized quadrupolar excitations in the spin-anisotropic frustrated magnet FeI 2

Magnetic order is usually associated with well-defined magnon excitations. Exotic magnetic fluctuations with fractional, topological or multipolar character, have been proposed for radically different forms of magnetic matter such as spin-liquids. As a result, considerable efforts have searched for, and uncovered, low-spin materials with suppressed dipolar order at low temperatures. In this work, we report neutron-scattering experiments and quantitative theoretical modeling of an exceptional spin-1 system – the uniaxial triangular magnet FeI 2 – where a bright and dispersive band of mixed dipolarquadrupolar fluctuations emerges just above a dipolar ordered ground-state. This excitation arises from anisotropic exchange interactions that hybridize overlapping modes carrying fundamentally different quantum numbers. Remarkably, a generalization of spin-wave theory to local SU(3) degrees of freedom accounts for all details of the low-energy dynamical response of FeI 2 without going beyond quadratic order. Our work highlights that quantum excitations without classical counterparts can be realized even in presence of fully developed magnetic order.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Direct observation of two-dimensional magnons in atomically thin CrI 3

Magnons are collective spin excitations in crystals with long-range magnetic order. The emergent van der Waals magnets provide a highly tunable platform to explore magnetic excitations in the two-dimensional limit with intriguing properties, manifesting from their honeycomb lattice structure and switchable magnetic configurations. Here, we report the direct observation of two-dimensional magnons through magneto-Raman spectroscopy with optical selection rules determined by the interplay between crystal symmetry, layer number and magnetic states in atomically thin CrI 3 . In monolayers, we observe an acoustic magnon mode at ~0.3 meV. It has strict cross-circularly polarized selection rules locked to the magnetization direction that originates from the conservation of angular momentum of photons and magnons dictated by three-fold rotational symmetry. Additionally, we reveal optical magnon modes at ~17 meV. This mode is Raman silent in monolayers, but optically active in bilayers and bulk due to a relaxation of the parity criterion resulting from the layer index. In the layered antiferromagnetic states, we directly resolve two degenerate optical magnon modes with opposite angular momentum and conjugate optical selection rules. From these measurements, we quantitatively extract the spin-wave gap, magnetic anisotropy and intralayer and interlayer exchange constants, and establish two-dimensional magnets as a new platform for exploring magnon physics.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Observing differential spin currents by resonant inelastic X-ray scattering

Controlling spin currents, that is, the flow of spin angular momentum, in small magnetic devices, is the principal objective of spin electronics, a main contender for future energy-efficient information technologies. A pure spin current has never been measured directly because the associated electric stray fields and/or shifts in the non-equilibrium spin-dependent distribution functions are too small for conventional experimental detection methods optimized for charge transport. Here we report that resonant inelastic X-ray scattering (RIXS) can bridge this gap by measuring the spin current carried by magnons—the quanta of the spin wave excitations of the magnetic order—in the presence of temperature gradients across a magnetic insulator. This is possible due to the sensitivity of the momentum- and energy-resolved RIXS intensity to minute changes in the magnon distribution under non-equilibrium conditions. Furthermore, we use the Boltzmann equation in the relaxation time approximation to extract transport parameters, such as the magnon lifetime at finite momentum, essential for the realization of magnon spintronics.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Single-shot electrical detection of short-wavelength magnon pulse transmission in a magnonic thin-film waveguide

Abstract The advance of magnon spintronics requires understanding of time-domain magnon pulse transmission in order to develop high-speed information processing protocols. In this work, we demonstrate single-shot electrical detection of narrow-band magnon pulse transmission in a yttrium iron garnet thin-film delay line. The high signal-to-background ratio of magnon transmission band allows us to directly probe the magnon transmission electrically using a fast oscilloscope and to study its spectral evolution using Fast Fourier Transform (FFT) of the time-domain transmitted signal. At elevated input power, we show a magnon transmission reduction and a spectral distortion, which can be understood by the nonlinear magnon excitation in the transmission band defined by the antenna geometry. In addition, we also find that the higher- (lower-) frequency magnon spectral component exhibits a lower (higher) magnon group velocity, showing a dispersion agreeing with the Damon-Eshbach dependence. Our results provide important guidance of magnon pulse engineering for their applications in spin wave computing and coherent magnon information processing.

Song, Moojune↗

DOE OSTI2025

Probing polarization-tunable sub-terahertz spin pumping in bimodal α-Fe 2 O 3 /Pt

Hematite (α-Fe 2 O 3 ) is an insulating antiferromagnet possessing a room temperature canted phase induced by the super-exchange Dzyaloshinskii-Moriya Interaction (DMI), resulting in enhanced spin pumping and spin transport over uniaxial antiferromagnets. In this work we resonantly excite the quasi-ferromagnetic (acoustic) and purely antiferromagnetic (optical) spin-dynamical modes in bulk and thin-film heterostructures of α-Fe 2 O 3 /Pt at room temperature, inducing inverse-spin-Hall-voltages up to 255 GHz. Following recent measurements of optical-mode spin-pumping in α-Fe 2 O 3 , we observe a novel and exotic microwave polarization mapping along with amplified spin-charge conversion in the optical branch and discuss the implications of layer thickness on acoustic and optical spin-modes. The results provide a deeper understanding of spin-wave selection rules for canted antiferromagnets and their potential use in nanoscale terahertz spintronics.

interfaces↗

DOE OSTI2022

NaCo 2 (SeO 3 ) 2 (OH): competing magnetic ground states of a new sawtooth structure with 3d 7 Co 2+ ions

While certain magnetic sublattices have long been known theoretically to give rise to emergent physics via competing magnetic interactions and quantum effects, finding such configurations in real materials is often deeply challenging. Here we report the synthesis and characterization of a new such material, NaCo 2 (SeO 3 ) 2 (OH) which crystallizes with a highly frustrated sublattice of sawtooth Co 2+ chains. Single crystals of NaCo 2 (SeO 3 ) 2 (OH) were synthesized using a low-temperature hydrothermal method. X-ray single crystal structure analysis reveals that the material crystallizes in orthorhombic space group of Pnma (no. 62). Its crystal structure exhibits one-dimensional chains of corner-sharing isosceles triangles that are made of two crystallographically distinct 3d 7 Co 2+ sites (Co(1) and Co(2)). The chains run along the b-axis and are interconnected via [SeO 3 ] groups to form a three-dimensional structure mediating super-exchange interactions. The temperature dependent magnetization data show a ferromagnetic-like (FM) transition at 11 K (T 1 ) followed by an antiferromagnetic (AFM) transition at about 6 K (T 2 ). Neutron-powder diffraction measurements reveal that at T 1 = 11 K only the Co(2) site orders magnetically, forming ferromagnetic zigzag chains along the b-axis. Below T 2 = 6 K, both Co(1) and Co(2) sites order in a nearly orthogonal configuration, with Co(1) moments lying inside the plane of the sawtooth chain while Co(2) moments cant out of the plane. The canting of the magnetic moments leads to a net ferromagnetic component along b-axis, parallel to the chain direction. The ordered moments are fully compensated in the ac-plane. Inelastic neutron scattering measurements reveal crystal field excitations that are consistent with the presence of a spin–orbital entangled pseudo-spin state J eff = 1/2 for the Co 2+ ions. Low-energy spin-wave excitations are observed below the second magnetic transition. The analysis of powder excitation spectrum suggests complex exchange interactions that go beyond a Heisenberg Hamiltonian model with nearest neighbor couplings. Our results demonstrate the richness of the magnetic properties of sawtooth-type structures and encourage the study of similar structures with different oxyanion groups.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2014

Electric field driven magnetic domain wall motion in ferromagnetic-ferroelectric heterostructures

We investigate magnetic domain wall (MDW) dynamics induced by applied electric fields in ferromagnetic-ferroelectric thin-film heterostructures. In contrast to conventional driving mechanisms where MDW motion is induced directly by magnetic fields or electric currents, MDW motion arises here as a result of strong pinning of MDWs onto ferroelectric domain walls (FDWs) via local strain coupling. By performing extensive micromagnetic simulations, we find several dynamical regimes, including instabilities such as spin wave emission and complex transformations of the MDW structure. In all cases, the time-averaged MDW velocity equals that of the FDW, indicating the absence of Walker breakdown.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Beyond Graphene: Low-Symmetry and Anisotropic 2D Materials

Low-symmetry 2D materials—such as ReS 2 and ReSe 2 monolayers, black phosphorus monolayers, group-IV monochalcogenide monolayers, borophene, among others—have more complex atomistic structures than the honeycomb lattices of graphene, hexagonal boron nitride, and transition metal dichalcogenides. The reduced symmetries of these emerging materials give rise to inhomogeneous electron, optical, valley, and spin responses, as well as entirely new properties such as ferroelasticity, ferroelectricity, magnetism, spin-wave phenomena, large nonlinear optical properties, photogalvanic effects, and superconductivity. Novel electronic topological properties, nonlinear elastic properties, and structural phase transformations can also take place due to low symmetry. Lastly, the “Beyond Graphene: Low-Symmetry and Anisotropic 2D Materials” Special Topic was assembled to highlight recent experimental and theoretical research on these emerging materials.

2D materials↗

DOE OSTI2023

Evaluation protocol for revealing magnonic contrast in TR-STXM measurements

We present a statistically motivated method to extract magnonic contrast from time-resolved scanning transmission x-ray microscopy (TR-STXM) measurements. TR-STXM is an element-specific method for resolving spin-dynamics in space and time. It offers nanometer spatial resolution and picosecond temporal resolution. The presented method makes it possible to obtain phase and amplitude profiles of spin-waves from STXM measurements. Furthermore, it allows for a rigorous transformation to reciprocal magnon k⃗-space, revealing k⃗-dependent magnon properties such as the magnon dispersion in three dimensions and for all directions of the magnetic anisotropy. We demonstrate our method using X-band ferromagnetic resonance on a micrometer-sized permalloy assembly.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Lithiating magneto-ionics in a rechargeable battery

Magneto-ionics, real-time ionic control of magnetism in solid-state materials, promise ultralow-power memory, computing, and ultralow-field sensor technologies. The real-time ion intercalation is also the key state-of-charge feature in rechargeable batteries. Here, we report that the reversible lithiation/delithiation in molecular magneto-ionic material, the cathode in a rechargeable lithium-ion battery, accurately monitors its real-time state of charge through a dynamic tunability of magnetic ordering. The electrochemical and magnetic studies confirm that the structural vacancy and hydrogen-bonding networks enable reversible lithiation and delithiation in the magnetic cathode. Coupling with microwave-excited spin wave at a low frequency (0.35 GHz) and a magnetic field of 100 Oe, we reveal a fast and reliable built-in magneto-ionic sensor monitoring state of charge in rechargeable batteries. The findings shown herein promise an integration of molecular magneto-ionic cathode and rechargeable batteries for real-time monitoring of state of charge.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Cobalt-based pyroxenes: A new playground for Kitaev physics

Recent advances in the study of cobaltites have unveiled their potential as a promising platform for realizing Kitaev physics in honeycomb systems and the Ising model in weakly coupled chain materials. In this manuscript, we explore the magnetic properties of pyroxene SrCoGe 2 O 6 using a combination of neutron scattering, ab initio methods, and linear spin-wave theory. Through careful examination of inelastic neutron scattering powder spectra, we propose a modified Kitaev model to accurately describe the twisted chains of edge-sharing octahedra surrounding Co 2+ ions. The extended Kitaev–Heisenberg model, including a significant anisotropic bond-dependent exchange term with K/|J| = 0.96, is identified as the key descriptor of the magnetic interactions in SrCoGe 2 O 6 . Furthermore, our heat capacity measurements reveal an effect of an external magnetic field (approximately 13 T) which shifts the system from a fragile antiferromagnetic ordering with T N = 9 K to a field-induced state. We argue that pyroxenes, particularly those modified by substituting Ge with Si and its less extended p orbitals, emerge as a platform for the Kitaev model. This opens up possibilities for advancing our understanding of Kitaev physics.

36 MATERIALS SCIENCE↗