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DOE OSTI2023

Skyrmion‐Excited Spin‐Wave Fractal Networks

Magnetic skyrmions exhibit unique, technologically relevant pseudo-particle behaviors which arise from their topological protection, including well-defined, 3D dynamic modes that occur at microwave frequencies. During dynamic excitation, spin waves are ejected into the interstitial regions between skyrmions, creating the magnetic equivalent of a turbulent sea. However, since the spin waves in these systems have a well-defined length scale, and the skyrmions are on an ordered lattice, ordered structures from spin-wave interference can precipitate from the chaos. This work uses small-angle neutron scattering (SANS) to capture the dynamics in hybrid skyrmions and investigate the spin-wave structure. Performing simultaneous ferromagnetic resonance and SANS, the diffraction pattern shows a large increase in low-angle scattering intensity, which is present only in the resonance condition. This scattering pattern is best fit using a mass fractal model, which suggests the spin waves form a long-range fractal network. The fractal structure is constructed of fundamental units with a size that encodes the spin-wave emissions and are constrained by the skyrmion lattice. Furthermore, these results offer critical insights into the nanoscale dynamics of skyrmions, identify a new dynamic spin-wave fractal structure, and demonstrate SANS as a unique tool to probe high-speed dynamics.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Molecular coupling competing with defects within insulator of the magnetic tunnel junction-based molecular spintronics devices

Nearly 70 years old dream of incorporating molecule as the device element is still challenged by competing defects in almost every experimentally tested molecular device approach. This paper focuses on the magnetic tunnel junction (MTJ) based molecular spintronics device (MTJMSD) method. An MTJMSD utilizes a tunnel barrier to ensure a robust and mass-producible physical gap between two ferromagnetic electrodes. MTJMSD approach may benefit from MTJ's industrial practices; however, the MTJMSD approach still needs to overcome additional challenges arising from the inclusion of magnetic molecules in conjunction with competing defects. Molecular device channels are covalently bonded between two ferromagnets across the insulating barrier. An insulating barrier may possess a variety of potential defects arising during the fabrication or operational phase. This paper describes an experimental and theoretical study of molecular coupling between ferromagnets in the presence of the competing coupling via an insulating tunnel barrier. We discuss the experimental observations of hillocks and pinhole-type defects producing inter-layer coupling that compete with molecular device elements. We performed theoretical simulations to encompass a wide range of competition between molecules and defects. Monte Carlo Simulation (MCS) was used for investigating the defect-induced inter-layer coupling on MTJMSD. Our research may help understand and design molecular spintronics devices utilizing various insulating spacers such as aluminum oxide (AlOx) and magnesium oxide (MgO) on a wide range of metal electrodes. This paper intends to provide practical insights for researchers intending to investigate the molecular device properties via the MTJMSD approach and do not have a background in magnetic tunnel junction fabrication.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Quantum Monte Carlo and Density Functional Theory Study of Strain and Magnetism in 2D 1T-VSe 2 with Charge Density Wave States

Two-dimensional (2D) 1T-VSe 2 has prompted significant interest due to the discrepancies regarding alleged ferromagnetism (FM) at room temperature, charge density wave (CDW) states, and the interplay between the two. We employed a combined Diffusion Monte Carlo (DMC) and density functional theory (DFT) approach to accurately investigate the magnetic properties, CDW states, and their responses to strain in monolayer 1T-VSe 2 . Our calculations show the delicate competition between various phases, revealing critical insights into the relationship between their energetic and structural properties. Here, we performed classical Monte Carlo simulations informed by our DMC and DFT results and found the magnetic transition temperature (T c ) of the undistorted (non-CDW) FM phase to be 228 K and the distorted (CDW) phase to be 68 K. Additionally, we studied the response of biaxial strain on the energetic stability and magnetic properties of various phases of 2D 1T-VSe 2 and found that small amounts of strain can increase the T c , suggesting a promising route for engineering and enhancing magnetic behavior. Finally, we synthesized 1T-VSe 2 and performed Raman spectroscopy measurements, which were in close agreement with our calculated results, validating our computational approach. Our work emphasizes the role of highly accurate DMC methods in advancing the understanding of monolayer 1T-VSe 2 and provides a robust framework for future studies of 2D magnetic materials.

2D magnets↗
DOE OSTI2021

Doping- and Strain-Dependent Electrolyte-Gate-Induced Perovskite to Brownmillerite Transformation in Epitaxial La 1– x Sr x CoO 3–δ Films

Much recent attention has focused on the voltage-driven reversible topotactic transformation between the ferromagnetic metallic perovskite (P) SrCoO 3-δ and oxygen-vacancy-ordered antiferromagnetic insulating brownmillerite (BM) SrCoO 2.5 . This is emerging as a paradigmatic example of the power of electrochemical gating (using, e.g., ionic liquids/gels), the wide modulation of electronic, magnetic, and optical properties generating clear application potential. SrCoO 3 films are challenging with respect to stability, however, and there has been little exploration of alternate compositions. Here, we present the first study of ion-gel-gating-induced P. BM transformations across almost the entire La 1-x SrxCoO 3 phase diagram (0 ≤ x ≤ 0.70), under both tensile and compressive epitaxial strain. Electronic transport, magnetometry, and operando synchrotron X-ray diffraction establish that voltage-induced P → BM transformations are possible at essentially all x, including x ≤ 0.50, where both P and BM phases are highly stable. Under small compressive strain, the transformation threshold voltage decreases from approximately +2.7 V at x = 0 to negligible at x = 0.70. Both larger compressive strain and tensile strain induce further threshold voltage lowering, particularly at low x. The P → BM threshold voltage is thus tunable, via both composition and strain. At x = 0.50, voltage-controlled ferromagnetism, transport, and optical transmittance are then demonstrated, achieving Curie temperature and resistivity modulations of similar to 220 K and at least 5 orders of magnitude, respectively, and enabling estimation of the voltage-dependent Co valence. The results are analyzed in the context of doping- and strain-dependent oxygen vacancy formation energies and diffusion coefficients, establishing that it is thermodynamic factors, not kinetics, that underpin the decrease in the threshold voltage with x, that is, with increasing formal Co valence. These findings substantially advance the practical and mechanistic understanding of this voltage-driven transformation, with fundamental and technological implications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Electric control of a canted-antiferromagnetic Chern insulator

Abstract The interplay between band topology and magnetism can give rise to exotic states of matter. For example, magnetically doped topological insulators can realize a Chern insulator that exhibits quantized Hall resistance at zero magnetic field. While prior works have focused on ferromagnetic systems, little is known about band topology and its manipulation in antiferromagnets. Here, we report that MnBi 2 Te 4 is a rare platform for realizing a canted-antiferromagnetic (cAFM) Chern insulator with electrical control. We show that the Chern insulator state with Chern number C = 1 appears as the AFM to canted-AFM phase transition happens. The Chern insulator state is further confirmed by observing the unusual transition of the C = 1 state in the cAFM phase to the C = 2 orbital quantum Hall states in the magnetic field induced ferromagnetic phase. Near the cAFM-AFM phase boundary, we show that the dissipationless chiral edge transport can be toggled on and off by applying an electric field alone. We attribute this switching effect to the electrical field tuning of the exchange gap alignment between the top and bottom surfaces. Our work paves the way for future studies on topological cAFM spintronics and facilitates the development of proof-of-concept Chern insulator devices.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Entangled core/shell magnetic structure driven by surface magnetic symmetry-breaking in Cr 2 O 3 nanoparticles

Bulk Cr 2 O 3 is an antiferromagnetic (AFM) oxide that exhibits the magnetoelectric effect at room temperature, with neither spontaneous magnetization nor net electric polarization. These physical properties stem from a subtle competition between exchange and crystal field interactions. In this article, we exploit the symmetry breaking at the surface of Cr 2 O 3 nanoparticles for unbalancing this delicate physical equilibrium. The emerging weak ferromagnetic signal we observe persists up to near room temperature (≈ 270 K) at which the antiferromagnetic order disappears. In addition, an exchange-bias effect, that rapidly decreases on heating from low temperature up to 30 K, is resistant to thermal disorder above 200 K. In conclusion, our findings point to the possible formation of an entangled core/shell magnetic structure, where pinned uncompensated spins at the shell are randomly distributed in a low-temperature spin-glass ordering, with low net magnetic moment and an ordering temperature governed by the AFM Néel temperature.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Mechanisms of Hysteresis and Reversibility across the Voltage-Driven Perovskite–Brownmillerite Transformation in Electrolyte-Gated Ultrathin La 0.5 Sr 0.5 CoO 3−δ

Perovskite cobaltites have emerged as archetypes for electrochemical control of materials properties in electrolyte-gate devices. Voltage-driven redox cycling can be performed between fully oxygenated perovskite and oxygen-vacancy-ordered brownmillerite phases, enabling exceptional modulation of the crystal structure, electronic transport, thermal transport, magnetism, and optical properties. The vast majority of studies, however, have focused heavily on the perovskite and brownmillerite end points. In contrast, here we focus on hysteresis and reversibility across the entire perovskite ↔ brownmillerite topotactic transformation, combining gate-voltage hysteresis loops, minor hysteresis loops, quantitative operando synchrotron X-ray diffraction, and temperature-dependent (magneto)transport, on ion-gel-gated ultrathin (10-unit-cell) epitaxial La 0.5 Sr 0.5 CoO 3-δ films. Further, gate-voltage hysteresis loops combined with operando diffraction reveal a wealth of new mechanistic findings, including asymmetric redox kinetics due to differing oxygen diffusivities in the two phases, nonmonotonic transformation rates due to the first-order nature of the transformation, and limits on reversibility due to first-cycle structural degradation. Minor loops additionally enable the first rational design of an optimal gate-voltage cycle. Combining this knowledge, we demonstrate state-of-the-art nonvolatile cycling of electronic and magnetic properties, encompassing >10 5 transport ON/OFF ratios at room temperature, and reversible metal-insulator-metal and ferromagnet-nonferromagnet-ferromagnet cycling, all at 10-unit-cell thickness with high room-temperature stability. This paves the way for future work to establish the ultimate cycling frequency and endurance of such devices.

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

Tablelike magnetocaloric effect and enhanced refrigerant capacity in EuO 1- δ thin films

The effect of electron doping of EuO 1- δ thin films through oxygen vacancies ( δ = 0, 0.025, and 0.09) upon the magnetocaloric response is presented here. The films each showed a paramagnetic to ferromagnetic transition around 65 K, with an additional magnetic ordering transition at higher temperatures in the oxygen deficient samples. All transitions are observed to be of second order. A maximum magnetic entropy change of 6.4 J/kg K over a field change of 2 T with a refrigerant capacity of 223 J/kg was found in the sample with δ = 0, and in all cases the refrigerant capacities of the thin films under study were found to exceed that reported for bulk EuO. Adjusting the oxygen content was shown to produce tablelike magnetocaloric effects, desirable for ideal Ericsson-cycle magnetic refrigeration. These films are thus excellent candidates for small-scale magnetic cooling technology in the liquid nitrogen temperature range.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Observation of novel charge ordering and spin reorientation in perovskite oxide PbFeO 3

Pb M O 3 ( M = 3 d transition metals) family shows systematic variations in charge distribution and intriguing physical properties due to its delicate energy balance between Pb 6 s and transition metal 3 d orbitals. However, the detailed structure and physical properties of PbFeO 3 remain unclear. Herein, we reveal that PbFeO 3 crystallizes into an unusual 2 a p × 6 a p × 2 a p orthorhombic perovskite super unit cell with space group Cmcm . The distinctive crystal construction and valence distribution of Pb 2+ 0.5 Pb 4+ 0.5 FeO 3 lead to a long range charge ordering of the -A-B-B- type of the layers with two different oxidation states of Pb (Pb 2+ and Pb 4+ ) in them. A weak ferromagnetic transition with canted antiferromagnetic spins along the a -axis is found to occur at 600 K. In addition, decreasing the temperature causes a spin reorientation transition towards a collinear antiferromagnetic structure with spin moments along the b -axis near 418 K. Our theoretical investigations reveal that the peculiar charge ordering of Pb generates two Fe 3+ magnetic sublattices with competing anisotropic energies, giving rise to the spin reorientation at such a high critical temperature.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Quasi-two-dimensional ferromagnetism and anisotropic interlayer couplings in the magnetic topological insulator MnBi 2 Te 4

MnBi 2 Te 4 (MBT) is a promising van der Waals layered antiferromagnetic (AFM) topological insulator that combines a topologically nontrivial inverted Bi-Te band gap with ferromagnetic (FM) layers of Mn ions. Here, the inelastic neutron scattering on single crystals reported here describes rather complex magnetism in MBT. The magnetic anisotropy that controls the bulk and surface magnetic field response of MBT is found to have contributions from both single-ion and interlayer two-ion terms. A description of the quasi-two-dimensional intralayer FM spin waves requires long-range, competing FM and AFM interactions and anomalous damping. While this might suggest carrier-mediated magnetic coupling, abinitio calculations in insulating MBT also find long-range interactions, and classical spin dynamics simulations suggest that magnetic vacancies are at least partially responsible for observations of anomalous damping near the zone boundary.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Trions in twisted bilayer graphene

The strong-coupling phase diagram of magic-angle twisted bilayer graphene (TBG) predicts a series of exact one-particle charge ±1 gapped excitations on top of the integer-filled ferromagnetic ground states. Finite-size exact diagonalization studies showed that these are the lowest charge ±1 excitations in the system (for 10 nm screening length), with the exception of charge +1 at filling -1 in the chiral limit. In the current paper we show that this “trion bound state,” a 3-particle, charge 1 excitation of the insulating ferromagnetic ground state of the projected Hamiltonian of TBG, is the lowest charge +1 overall excitation at ν =-1, and also for some large (≈20 nm) screening lengths at ν =-2 in the chiral limit and with very small binding energy. At other fillings, we show that trion bound states do exist, but only for momentum ranges that do not cover the entire moiré Brillouin zone. The trion bound states (at different momenta) exist for finite parameter range w 0 /w 1 but they all disappear in the continuum far below the realistic values of w 0 /w 1 = 0.8. Thus we find the conditions for the existence of the trion bound state, a good variational wave function for it, and investigate its behavior for different screening lengths, at all integer fillings, on both the electron and hole sides.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Low-Field EMR Studies of Permalloy Films and Gratings

Flat and profile-modulated permalloy films have been studied by the electron magnetic resonance (EMR) method. In addition to ferromagnetic and spin-wave resonances, the structures demonstrate low-field EMR signals of an unusual shape, which form a hysteresis loop in sweeping fields. The low-field signals are attributed to a fast reorientation of magnetic domains. The low-field EMR behavior is comparable to the behavior in magneto-dependent photovoltage previously observed in the optical experiments. The shapes of the loops and typical values of the switching fields depend on the profile modulation parameters confirming the possibility of controlling magnetic properties and the coupling of magnetic and optical effects with nanoscale geometry.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Anomalous and planar Hall effects in Co 1−x Ho x thin films across the magnetic sublattice compensation temperature

Metallic amorphous ferrimagnets derived from alloying 3d transition metals with 4f-electron rare earths host fascinating effects of compensation between the 3d and 4f magnetic sublattices. Here, a detailed study of the anisotropic magnetoresistance (Δρ xx ), planar Hall effect (ρ xy PHE ), and anomalous Hall effect (ρ xy AHE ) is reported on a series of Co 1−x Ho x thin films over a wide field–temperature (H–T) phase space. Close to the magnetic compensation temperature, the ρ xy AHE –H loops show a double sign reversal and signatures of spin-flop transition at higher fields. The Δρ xx and ρ xy PHE also display strong deviations from the classical angular dependence seen in soft ferromagnets like permalloy as the angle ϕ between in-plane current and magnetic field is scanned from 0 to 2π. It is argued that the non-zero orbital angular momentum of Ho ions in the lattice and stabilization of bubble domains below magnetic saturation may be responsible for such features. Direct imaging of magnetic textures with x-ray photoelectron microscopy shows the formation of stripe domain patterns in the regime of sublattice compensation. Such stripes are likely to transform into magnetic bubbles before full saturation is reached in a large magnetic field.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Unraveling the nature of Fe-doping mediated inter- and intra-chain interactions in Ca 3 Co 2 O 6

The structural and magnetic properties of quasi-one-dimensional (1D) spin-chain compounds Ca 3 Co 2-x Fe x O 6 (x = 0, 0.1, 0.2 and 0.3) synthesized by a sol-gel method have been systematically studied by means of X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), neutron powder diffraction (NPD), dc and ac magnetization measurements. The samples adopt a rhombohedral crystal structure with the space group R-3c in a temperature range of 5–100 K. Fe ions are found to locate at the trigonal prism Co2 crystallographic sites. Fe doping converts some of low-spin Co 3+ ions at Co1 octahedral sites into Co 2+ ions. For the high-temperature paramagnetic phase, the Curie paramagnetic temperature θp changes its sign from positive to negative at x = 0.2, implying that the dominant magnetic interaction is driven from ferromagnetic (FM) to antiferromagnetic (AFM) upon Fe substitution. A partial low-spin to high-spin state crossover of the Co1 ions is observed at high Fe-doping level x = 0.3. All the samples exhibit a long-range spin-density wave (SDW) AFM ordering below TN, followed by a spin-glass-like transition at Tf. These low-temperature magnetic phases were significantly suppressed upon Fe doping. The Fe substitution in Ca 3 Co 2-x Fe x O 6 weakened both intrachain and interchain magnetic interactions, caused by enhanced magnetic disorder due to the different magnetic characters of Ising Co and Heisenberg Fe spins.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Capturing the ground state of uranium dioxide from first principles: Crystal distortion, magnetic structure, and phonons

Uranium dioxide (UO 2 ) remains a formidable challenge for first-principles approaches due to the complex interplay among spin-orbit coupling, Mott physics, magnetic ordering, and crystal distortions. Here we use DFT+U to explore UO 2 at zero temperature, incorporating all the aforementioned phenomena. The technical challenge is to navigate the many metastable electronic states produced by DFT+U, which is accomplished using f-orbital occupation matrix control to search for the ground state. We restrict our search to the high-symmetry ferromagnetic phase, including spin-orbit coupling, which produces a previously unreported occupation matrix. This newfound occupation matrix is then used as an initialization to explore the broken symmetry phases. We find the oxygen cage distortion of the 3k antiferromagnetic state to be in excellent agreement with experiments, and both the spin-orbit coupling and the Hubbard U are critical ingredients. Further, we demonstrate that only select phonon modes have a strong dependence on the Hubbard U, whereas magnetic ordering has only a small influence overall. We perform measurements of the phonon dispersion curves using inelastic neutron scattering, and our calculations show good agreement when using reasonable values of U. The quantitative success of DFT+U warrants exploration of thermal transport and other observables within this level of theory.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Magnetic phase transitions in Eu(Co 1-x Nix) 2-y As 2 single crystals

The effects of Ni doping in Eu(Co 1-x Ni x ) 2-y As 2 single crystals with x = 0 to 1 grown out of self flux are investigated via crystallographic, electronic transport, magnetic, and thermal measurements. All compositions adopt the body-centered-tetragonal ThCr 2 Si 2 structure with space group I 4= mmm . Here, we also find 3-4% of randomly-distributed vacancies on the Co/Ni site. Anisotropic magnetic susceptibility $\chi$α (α = ab; c) data versus temperature T show clear signatures of an antiferromagnetic (AFM) c-axis helix structure associated with the Eu +2 spins-7/2 for x = 0 and x = 1 as previously reported. The $\chi$α (T) data for x = 0.03 and 0.10 suggest an anomalous 2 q magnetic structure containing two helix axes along the c axis and in the ab plane, respectively, whereas for x = 0.75, 0.82, and 1 a c-axis helix is inferred as previously found for x = 1. At intermediate compositions x = 0:2, 0.32, 0.42, 0.54, and 0.65 a magnetic structure with a large ferromagnetic (FM) c-axis component is found from magnetization versus fi eld isotherms, suggested to be an incommensurate FM cone structure associated with the Eu spins, which consists of both AFM and FM components. In addition, the $\chi$ (T) and heat capacity C p (T) data for x = 0.2-0.65 indicate the occurrence of itinerant FM order associated with the Co/Ni atoms with Curie temperatures from 60 K to 25 K, respectively. Electrical resistivity ρ(T) measurements indicate metallic character for all compositions with abrupt increases in slope on cooling below the Eu AFM transition temperatures. In addition to this panoply of magnetic transitions, 151 Eu Mössbauer measurements indicate that ordering of the Eu moments proceeds via an incommensurate sine amplitude-modulated structure with additional transition temperatures associated with this effect.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Magnetic properties of (Mo 2/3 Dy 1/3 ) 2 AlC arc melted polycrystalline samples

Here, this study investigates the structural and magnetic properties of arc-melted (Mo 2/3 Dy 1/3 ) 2 AlC polycrystalline samples, a member of the i-MAX phase family. Temperature-dependent magnetization and specific heat measurements confirm the low-temperature antiferromagnetic transitions around 14 K and 17 K. Neutron diffraction data collected at 4 K reveal the emergence of magnetic Bragg peaks that are not allowed in the paramagnetic space group C2/c, further confirming the presence of antiferromagnetic ordering. The detection of a secondary phase, DyAl 2 , is complicated by overlapping Bragg peaks with the monoclinic phase of (Mo 2/3 Dy 1/3 ) 2 AlC in powder XRD patterns. However, magnetization and neutron diffraction data suggest the presence of DyAl 2 , evidenced by a ferromagnetic phase transition around 62 K.

36 MATERIALS SCIENCE↗
DOE OSTI2021

String Phase in an Artificial Spin Ice

Abstract One-dimensional strings of local excitations are a fascinating feature of the physical behavior of strongly correlated topological quantum matter. Here we study strings of local excitations in a classical system of interacting nanomagnets, the Santa Fe Ice geometry of artificial spin ice. We measured the moment configuration of the nanomagnets, both after annealing near the ferromagnetic Curie point and in a thermally dynamic state. While the Santa Fe Ice lattice structure is complex, we demonstrate that its disordered magnetic state is naturally described within a framework of emergent strings. We show experimentally that the string length follows a simple Boltzmann distribution with an energy scale that is associated with the system’s magnetic interactions and is consistent with theoretical predictions. The results demonstrate that string descriptions and associated topological characteristics are not unique to quantum models but can also provide a simplifying description of complex classical systems with non-trivial frustration.

36 MATERIALS SCIENCE↗