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DOE OSTI2024

Unconventional pressure-induced magnetic transitions and mechanical properties in non-magnetic LaFeSi

Here, this work demonstrates that two consecutive magnetic transitions occur in non-magnetic LaFeSi compound under negative hydrostatic pressure (small volume expansion). Electronic structure properties of LaFeSi were calculated using density functional theory (DFT) to understand the origin of these magnetic transitions. Mechanical properties of LaFeSi, especially elastic properties (shear and Young’s modulus, and Poisson’s ratio), were determined by DFT distortion calculations to elucidate lattice anisotropy and stability. The antiferromagnetic transition at –7.52 GPa, predicted in our work for LaFeSi, is consistent with the reported experimentally observed antiferromagnetic ground states in CeMnSi and LaMnSi compounds having similar crystal geometry. This finding of unexpected magnetic ordering predicts that layered non-magnetic materials, like LaFeSi, may become magnetically active with lattice expansion.

36 MATERIALS SCIENCE↗

DOE OSTI2015

Structural, magnetic and optical properties of a dilute magnetic semiconductor based on Ce{sub 1−x}Co{sub x}O{sub 2} thin film grown on LaAlO{sub 3}

Highlights: • Co doped CeO{sub 2} was grown on LaAlO{sub 3} (0 0 1) via a modified sol–gel spin-coating technique. • The concentration of the Co ions was varied from 1 to 15 at.%. • The incorporation of 5 at.% of Mn ions was found to provide formation of exceptionally magnetic moment. • This amount demonstrated a giant magnetic moment of 1.09 μ{sub B}/Co. • This amount reduced the optical band gap and enhanced the optical performance. - Abstract: The enhancement of the room temperature ferromagnetism and optical properties of the dilute magnetic metal oxides is a crucial clue to construct spin-based optoelectronic devices. In this work, Ce{sub 1−x}Co{sub x}O{sub 2} (0.01 ≤ x ≤0.15) thin films were prepared via ethylene glycol modified sol–gel spin coating technique on the LaAlO{sub 3} (0 0 1) substrate to enhance their room temperature ferromagnetism and optical properties. The structures, magnetic and optical properties of the prepared films were characterized by X-ray diffraction, atomic force microscopy, scanning electron microscopy, energy dispersive X-ray spectroscopy, SQUID magnetometer, X-ray photoelectron spectroscopy and UV–vis spectrophotometer. The results demonstrated that a single phase cubic structure was formed, implying the substitution of Co ions into the Ce ions sites. The prepared films showed room temperature ferromagnetism with saturation magnetic moment of 1.09 μ{sub B}/Co was achieved for 5 at.% Co-doped CeO{sub 2}. This film exhibited high optical transparency of 85% and low optical band energy gap of 3.39 eV. The improved magnetic and optical properties are argued to the increase of the density of the oxygen vacancies into the cerium oxide crystal structure due to the incorporation of Co ions.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Layer-Dependent Magnetism and Spin Fluctuations in Atomically Thin van der Waals Magnet CrPS 4

van der Waals (vdW) magnets, an emerging family of two-dimensional (2D) materials, have received tremendous attention due to their rich fundamental physics and significant potential for cutting-edge technological applications. In contrast to the conventional bulk counterparts, vdW magnets exhibit significant tunability of local material properties, such as stacking engineered interlayer coupling and layer-number dependent magnetic and electronic interactions, which promise to deliver previously unavailable merits to develop multifunctional microelectronic devices. As a further ingredient of this emerging topic, here we report nanoscale quantum sensing and imaging of atomically thin vdW magnet chromium thiophosphate CrPS 4 , revealing its characteristic layer-dependent 2D static magnetism and dynamic spin fluctuations. We also show a large tunneling magnetoresistance in CrPS 4 -based spin filter vdW heterostructures. Here, the excellent material stability, robust strategy against environmental degradation, in combination with tailored magnetic properties highlight the potential of CrPS 4 in developing state-of-the-art 2D spintronic devices for next-generation information technologies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Raman Shifts in Two-Dimensional van der Waals Magnets Reveal Magnetic Texture Evolution

Two-dimensional (2D) van der Waals magnets comprise rich physics that can be exploited for spintronic applications. We investigate the interplay between spin-phonon coupling and spin textures in a 2D van der Waals magnet by combining magneto-Raman spectroscopy with cryogenic Lorentz transmission electron microscopy. Here we find that when stable skyrmion bubbles are formed in the 2D magnet, a field-dependent Raman shift can be observed, and this shift is absent for the 2D magnet prepared in its ferromagnetic state. Correlating these observations with numerical simulations that take into account field-dependent magnetic textures and spin--phonon coupling in the 2D magnet, we associate the Raman shift to field-induced modulations of the skyrmion bubbles and derive the existence of inhomogeneity in the skyrmion textures over the film thickness.

2D van der Waals magnet↗

DOE OSTI2020

Proximity Spin–Orbit Torque on a Two-Dimensional Magnet within van der Waals Heterostructure: Current-Driven Antiferromagnet-to-Ferromagnet Reversible Nonequilibrium Phase Transition in Bilayer CrI 3

The recently discovered two-dimensional magnetic insulator CrI 3 is an intriguing case for basic research and spintronic applications since it is a ferromagnet in the bulk but an antiferromagnet in bilayer form, with its magnetic ordering amenable to external manipulations. Using the first-principles quantum transport approach, we predict that injecting unpolarized charge current parallel to the interface of the bilayer-CrI 3 /monolayer-TaSe 2 van der Waals (vdW) heterostructure will induce spin–orbit torque and thereby drive the dynamics of magnetization on the first monolayer of CrI 3 in direct contact with TaSe 2 . By combining the calculated complex angular dependence of spin–orbit torque with the Landau-Lifshitz-Gilbert equation for classical dynamics of magnetization, we demonstrate that current pulses can switch the direction of magnetization on the first monolayer to become parallel to that of the second monolayer, thereby converting CrI 3 from antiferromagnet to ferromagnet while not requiring any external magnetic field. We explain the mechanism of this reversible current-driven nonequilibrium phase transition by showing that first monolayer of CrI 3 carries current due to evanescent wave functions injected by metallic transition metal dichalcogenide TaSe 2 , while concurrently acquiring strong spin–orbit coupling via such a proximity effect, whereas the second monolayer of CrI 3 remains insulating. Furthermore, the transition can be detected by passing vertical read current through the vdW heterostructure, encapsulated by a bilayer of hexagonal boron nitride and sandwiched between graphite electrodes, where we find a tunneling magnetoresistance of ≃240%.

2D magnetic materials↗

DOE OSTI2022

Density Functional Theory Study of Controllable Optical Absorptions and Magneto-Optical Properties of Magnetic CrI 3 Nanoribbons: Implications for Compact 2D Magnetic Devices

A chromium triiodide (CrI 3 ) monolayer has an interesting ferromagnetic ground-state. In this work, we calculate band structures and magnetic moments of tensile-strained and bent zigzag CrI 3 nanoribbons with density functional theory. The edge iodine atoms form flat low-lying conduction bands and couple with chromium atoms ferromagnetically, while the non-edge iodine atoms weakly couple antiferromagnetically. Narrow CrI 3 nanoribbons have two locally stable magnetic moment orientations, namely out-of-plane and in-plane (along the nanoribbon periodic direction) configurations. This enables four magnetization states in CrI 3 nanoribbons, including two out-of-plane ones (up and down) and two in-plane ones (forward and backward along the nanoribbon periodical direction), increasing the operating controllability. Based on the one-dimensional Ising spin chain model, the spin correlation length of the narrow CrI 3 nanoribbon is estimated as about 10 Å at its estimated Curie temperature of 27 Kelvin, which is lower than the measured 45 Kelvin of the monolayer CrI 3 . The optical absorption and magneto-optical properties of CrI 3 nanoribbons are investigated with many-body perturbation GW-BSE (Bethe-Salpeter equation), including magnetic dichroism, Faraday and magneto-optical Kerr effects. Here, the low-energy dark excitons are mainly from transitions between electrons and holes with unlike spins and are non-Frenkel-like, while the bright excitons have mixed spin configurations. The intrinsic lifetime of excitons can be over one nanosecond, suitable for quantum information processes. Tensile strains and bending manifestly modulate the absorption spectra and magneto-optical properties of CrI 3 nanoribbons within a technologically important photon energy-range of ~1.0-2.0 eV. The CrI 3 nanoribbons can be used in 1D or 2D magnetic storage nanodevices, tunable magnetic optoelectronics, and spin-based quantum information controls.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Proximity-Induced Magnetic Order in a Transferred Topological Insulator Thin Film on a Magnetic Insulator

Breaking the time reversal symmetry (TRS) in a topological insulator (TI) by introducing a magnetic order gives rise to exotic quantum phenomena. One of the promising routes to inducing a magnetic order in a TI is utilizing magnetic proximity effect between a TI and a strong magnetic insulator (MI). Here, we demonstrate a TI/MI heterostructure prepared through transferring a molecular beam epitaxy (MBE)-grown Bi 2 Se 3 film onto a yttrium iron garnet (YIG) substrate via wet transfer. The transferred Bi 2 Se 3 exhibits excellent quality over a large scale. Moreover, through wet transfer we are able to engineer the interface and perform a comparative study to probe the proximity coupling between Bi 2 Se 3 and YIG under different interface conditions. A detailed investigation of both the anomalous Hall effect and quantum corrections to the conductivity in magnetotransport measurements reveals an induced magnetic order as well as TRS breaking in the transferred Bi 2 Se 3 film on YIG. In contrast, a thin layer of AlO x at the interface obstructs the proximity coupling and preserves the TRS, indicating the critical role of the interface in mediating magnetic proximity effect.

42 ENGINEERING↗

DOE OSTI2015

Revealing giant internal magnetic fields due to spin fluctuations in magnetically doped colloidal nanocrystals

Strong quantum confinement in semiconductors can compress the wavefunctions of band electrons and holes to nanometre-scale volumes, significantly enhancing interactions between themselves and individual dopants. In magnetically doped semiconductors, where paramagnetic dopants (such as Mn 2+ , Co 2+ and so on) couple to band carriers via strong sp–d spin exchange, giant magneto-optical effects can therefore be realized in confined geometries using few or even single impurity spins. Importantly, however, thermodynamic spin fluctuations become increasingly relevant in this few-spin limit. In nanoscale volumes, the statistical √N fluctuations of N spins are expected to generate giant effective magnetic fields B eff , which should dramatically impact carrier spin dynamics, even in the absence of any applied field. In this paper, we directly and unambiguously reveal the large B eff that exist in Mn 2+ -doped CdSe colloidal nanocrystals using ultrafast optical spectroscopy. At zero applied magnetic field, extremely rapid (300–600 GHz) spin precession of photoinjected electrons is observed, indicating B eff ~ 15-30 T for electrons. Precession frequencies exceed 2 THz in applied magnetic fields. Finally, these signals arise from electron precession about the random fields due to statistically incomplete cancellation of the embedded Mn 2+ moments, thereby revealing the initial coherent dynamics of magnetic polaron formation, and highlighting the importance of magnetization fluctuations on carrier spin dynamics in nanomaterials.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2024

Observation of stacking engineered magnetic phase transitions within moiré supercells of twisted van der Waals magnets

Abstract Recent demonstrations of moiré magnetism, featuring exotic phases with noncollinear spin order in the twisted van der Waals (vdW) magnet chromium triiodide CrI 3 , have highlighted the potential of twist engineering of magnetic (vdW) materials. However, the local magnetic interactions, spin dynamics, and magnetic phase transitions within and across individual moiré supercells remain elusive. Taking advantage of a scanning single-spin magnetometry platform, here we report observation of two distinct magnetic phase transitions with separate critical temperatures within a moiré supercell of small-angle twisted double trilayer CrI 3 . By measuring temperature-dependent spin fluctuations at the coexisting ferromagnetic and antiferromagnetic regions in twisted CrI 3 , we explicitly show that the Curie temperature of the ferromagnetic state is higher than the Néel temperature of the antiferromagnetic one by ~10 K. Our mean-field calculations attribute such a spatial and thermodynamic phase separation to the stacking order modulated interlayer exchange coupling at the twisted interface of moiré superlattices.

36 MATERIALS SCIENCE↗

DOE OSTI2014

Magnetization reversal induced by in-plane current in Ta/CoFeB/MgO structures with perpendicular magnetic easy axis

We investigate in-plane current-induced magnetization reversal under an in-plane magnetic field in Hall bar shaped devices composed of Ta/CoFeB/MgO structures with perpendicular magnetic easy axis. The observed relationship between the directions of current and magnetization switching and Ta thickness dependence of magnetization switching current are accordance with those for magnetization reversal by spin transfer torque originated from the spin Hall effect in the Ta layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2015

Magnetized sheath near positively biased wall between two permanent magnetic plates

The characteristics of magnetized electron sheath near a positively biased conducting wall parallel to magnetic field formed between two permanent magnetic plates were experimentally investigated in a double plasma device. The magnetic field strength between the magnetic plates is about 1200 G which is sufficient to magnetize the plasma such that the ion gyroradius is comparable to the electron Debye length. A virtual cathode (or potential dip) structure was found between the electron-rich sheath and bulk plasma. For a given neutral gas pressure, the potential minimum (dip position) remains almost the same for different positive biases on the wall. For a given bias on the wall, however, the electron sheath thickness and the potential drop from the bulk plasma to the dip decrease with the increase of the neutral gas pressure. In addition, the electron sheath and potential dip appear to be wider and deeper in the downstream side of the wall.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2015

Microwave soft x-ray microscopy for nanoscale magnetization dynamics in the 5–10 GHz frequency range

We present a scanning transmission x-ray microscopy setup combined with a novel microwave synchronization scheme for studying high frequency magnetization dynamics at synchrotron light sources. The sensitivity necessary to detect small changes in the magnetization on short time scales and nanometer spatial dimensions is achieved by combining the excitation mechanism with single photon counting electronics that is locked to the synchrotron operation frequency. Our instrument is capable of creating direct images of dynamical phenomena in the 5-10 GHz range, with high spatial resolution. When used together with circularly polarized x-rays, the above capabilities can be combined to study magnetic phenomena at microwave frequencies, such as ferromagnetic resonance (FMR) and spin waves. We demonstrate the capabilities of our technique by presenting phase resolved images of a ∼6 GHz nanoscale spin wave generated by a spin torque oscillator, as well as the uniform ferromagnetic precession with ∼0.1° amplitude at ∼9 GHz in a micrometer-sized cobalt strip.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2015

Quasi-discrete particle motion in an externally imposed, ordered structure in a dusty plasma at high magnetic field

Dusty plasmas have been studied in argon, radio frequency (rf) glow discharge plasmas at magnetic fields up to 2.5 T where the electrons and ions are strongly magnetized. Plasmas are generated between two parallel plate electrodes where the lower, powered electrode is solid and the upper electrode supports a dual mesh consisting of #24 brass and #30 aluminum wire cloth. In this experiment, we study the formation of imposed ordered structures and particle dynamics as a function of magnetic field. Through observations of trapped particles and the quasi-discrete (i.e., “hopping”) motion of particles between the trapping locations, it is possible to make a preliminary estimate of the potential structure that confines the particles to a grid structure in the plasma. In conclusion, this information is used to gain insight into the formation of the imposed grid pattern of the dust particles in the plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2015

Site preference and magnetic properties of Ga/In-substituted strontium hexaferrite: An ab initio study

The first-principles density functional theory has been used to study Ga/In-substituted strontium hexaferrite (SrFe12O19). Based on the calculation of the substitution energy of Ga and In in SrFe12O19 and the formation probability analysis, we conclude that in SrFe12−xGaxO19 the substituted Ga atoms prefer to occupy the 12k, 2a, and 4f1 sites, while In atoms in SrFe12−xInxO19 occupy the 12k, 4f2, and 4f1 sites. We used the site occupation probabilities to calculate the magnetic properties of the substituted SrFe12O19. It was found that as the fraction of Ga atoms in SrFe12−xGaxO19 increases, the saturation magnetization (Ms) as well as magnetic anisotropy energy (MAE) decrease, while the anisotropy field (Ha) increases. In the case of SrFe12−xInxO19, Ms, MAE, and Ha decrease with an increase of the concentration of In atoms.

Dixit, Vivek (ORCID:000000029178217X)↗

DOE OSTI2016

Effect of axial magnetic field on a 2.45 GHz permanent magnet ECR ion source

Herein, we conduct a fundamental study to improve the generation efficiency of a multi-charged ion source using argon. A magnetic field of our electron cyclotron resonance ion source is composed of a permanent magnet and a solenoid coil. Thereby, the axial magnetic field in the chamber can be tuned. Using the solenoid coil, we varied the magnetic field strength in the plasma chamber and measured the ion beam current extracted at the electrode. We observed an approximately three times increase in the Ar{sup 4+} ion beam current when the magnetic field on the extractor-electrode side of the chamber was weakened. From our results, we can confirm that the multi-charged ion beam current changes depending on magnetic field intensity in the plasma chamber.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2016

Effect of magnetic field on noncollinear magnetism in classical bilinear-biquadratic Heisenberg model

We present a Monte Carlo simulation study of a bilinear-biquadratic Heisenberg model on a two-dimensional square lattice in the presence of an external magnetic field. The study is motivated by the relevance of this simple model to the non-collinear magnetism and the consequent ferroelectric behavior in the recently discovered high-temperature multiferroic, cupric oxide (CuO). We show that an external magnetic field stabilizes a non-coplanar magnetic phase, which is characterized by a finite ferromagnetic moment along the direction of the applied magnetic field and a spiral spin texture if projected in the plane perpendicular to the magnetic field. Real-space analysis highlights a coexistence of non-collinear regions with ferromagnetic clusters. The results are also supported by simple variational calculations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2016

Extended magnetic exchange interactions in the high-temperature ferromagnet MnBi

The high-temperature ferromagnet MnBi continues to receive attention as a candidate to replace rare-earth-containing permanent magnets in applications above room temperature. This is due to a high Curie temperature, large magnetic moments, and a coercivity that increases with temperature. The synthesis of MnBi also allows for crystals that are free of interstitial Mn, enabling more direct access to the key interactions underlying the physical properties of binary Mn-based ferromagnets. In this work, we use inelastic neutron scattering to measure the spin waves of MnBi in order to characterize the magnetic exchange at low temperature. Consistent with the spin reorientation that occurs below 140 K, we do not observe a spin gap in this system above our experimental resolution. A Heisenberg model was fit to the spin wave data in order to characterize the long-range nature of the exchange. It was found that interactions up to sixth nearest neighbor are required to fully parametrize the spin waves. Surprisingly, the nearest-neighbor term is antiferromagnetic, and the realization of a ferromagnetic ground state relies on the more numerous ferromagnetic terms beyond nearest neighbor, suggesting that the ferromagnetic ground state arises as a consequence of the long-ranged interactions in the system.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

Magnetically tunable unidirectional waveguide based on magnetic photonic crystals

In this letter, we presented a magnetically tunable ferrite-loaded unidirectional waveguide based on magnetic photonic crystals. Two rows of ferrite rods are symmetrically arranged near the two lateral sides of the rectangular waveguide, where they are biased with static magnetic fields with the same amplitude and opposite directions along the rod axis. Since the magnetic one-way transmission is induced by the magnetic surface plasmon resonance, the operating band of the unidirectional waveguide can be tuned by changing the biased magnetic field intensity. To validate the design, a prototype was fabricated and measured. Both the simulation and experiment results verify the unidirectional transmission property.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗