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DOE OSTI2020

Prediction of room-temperature multiferroicity in strained MoCr 2 S 6 monolayer

The contrasting d-orbital occupation required for ferroelectricity vs ferromagnetism makes it difficult for their coexistence in two-dimensional materials, especially at high temperature. To resolve this intrinsic contradiction, we propose a layered MoCr 2 S 6 multiferroics by alloying magnetic Cr element into the ferroelectric 1T phase of the MoS 2 matrix. First-principles calculations disclose that a spontaneous symmetry breaking, depending on the Mo atom displacement, leads to a robust ferroelectricity, which coexists with a ferromagnetic order originated from two neighboring Cr atoms. The effect can be further enhanced by tensile strain to bring about a room-temperature multiferroicity. Our results shed new light on the fundamental understanding of multiferroics and display promising applications in spintronics and multistate data storage.

2D materials↗

DOE OSTI2020

Synthetic antiferromagnet-based spin Josephson oscillator

Two easy-plane ferromagnetic layers, antiferromagnetically coupled through a thin nonmagnetic metal layer, form the magnetic analog of a Josephson junction. Additionally, a current driven spin chemical potential drives a 2π precession of the in-plane magnetization of each ferromagnet. The participation of the full magnetic moment in the 2π precession maximizes the giant magnetoresistance and the ac output power. The frequency can be continuously tuned by a dc bias. An applied ac bias results in a time-averaged magnetoresistance with Shapiro-like steps. The multistate mode-locking behavior exhibited by the Shapiro steps may be exploited for applications such as microwave detectors and neuromorphic computing. They may also serve as an experimental signature of spin superfluidity.

42 ENGINEERING↗

DOE OSTI2020

Light induced electron spin resonance properties of van der Waals CrX 3 (X = Cl, I) crystals

The research on layered van der Waals (vdW) magnets is rapidly progressing owing to exciting fundamental science and potential applications. In bulk crystal form, CrCl 3 is a vdW antiferromagnet with in-plane ferromagnetic ordering below 17 K, and CrI 3 is a vdW ferromagnet below 61 K. In this paper, we report on the electron spin resonance (ESR) properties of CrCl 3 and CrI 3 single crystals upon photo-excitation in the visible range. We noticed remarkable changes in the ESR spectra upon illumination. In the case of CrCl 3 , at 10 K, the ESR signal is shifted from g = 1.492 (dark) to 1.661 (light), the linewidth increased from 376 to 506 Oe, and the signal intensity is reduced by 1.5 times. Most interestingly, the observed change in the signal intensity is reversible when the light is cycled on/off. We observed almost no change in the ESR spectral parameters in the paramagnetic phase (>20 K) upon illumination. Upon photo-excitation of CrI 3 , the ESR signal intensity is reduced by 1.9 times; the g-value increased from 1.956 to 1.990; the linewidth increased from 1170 to 1260 Oe at 60 K. These findings are discussed by taking into account the skin depth, the slow relaxation mechanism, and the appearance of low-symmetry fields at the photo-generated Cr 2+ Jahn–Teller centers. Such an increase in the g-value as a result of photo-generated Cr 2+ ions is further supported by our many-body wavefunction calculations. This work has the potential to extend to monolayer vdWs magnets by combining ESR spectroscopy with optical excitation and detection.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

Interfacial spin–orbit torques

Spin–orbit torques offer a promising mechanism for electrically controlling magnetization dynamics in nanoscale heterostructures. While spin–orbit torques occur predominately at interfaces, the physical mechanisms underlying these torques can originate in both the bulk layers and at interfaces. Classifying spin–orbit torques based on the region that they originate in provides clues as to how to optimize the effect. While most bulk spin–orbit torque contributions are well studied, many of the interfacial contributions allowed by symmetry have yet to be fully explored theoretically and experimentally. To facilitate progress, we review interfacial spin–orbit torques from a semiclassical viewpoint and relate these contributions to recent experimental results. In this study, we show the relationship between different interface transport parameters within the same model. For charges and spins flowing perpendicular to the interface, interfacial spin–orbit coupling both modifies the mixing conductance of the magnetoelectronic circuit theory and gives rise to spin memory loss. For in-plane electric fields, interfacial spin–orbit coupling gives rise to torques described by spin–orbit filtering, spin swapping, and precession. In addition, these same interfacial processes generate spin currents that flow into the non-magnetic layer. For in-plane electric fields in trilayer structures, the spin currents generated at the interface between one ferromagnetic layer and the non-magnetic spacer layer can propagate through the non-magnetic layer to produce novel torques on the other ferromagnetic layer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Magnetic imaging and statistical analysis of the metamagnetic phase transition of FeRh with electron spins in diamond

Magnetic imaging based on nitrogen-vacancy (NV) centers in diamond has emerged as a powerful tool for probing magnetic phenomena in fields ranging from biology to physics. A key strength of NV sensing is its local-probe nature, enabling high-resolution spatial images of magnetic stray fields emanating from a sample. However, this local character can also form a drawback for analyzing the global properties of a system, such as a phase transition temperature. Here, we address this challenge by using statistical analyses of magnetic-field maps to characterize the first-order temperature-driven metamagnetic phase transition from the antiferromagnetic to the ferromagnetic state in FeRh. After imaging the phase transition and identifying the regimes of nucleation, growth, and coalescence of ferromagnetic domains, we statistically characterize the spatial magnetic-field maps to extract the transition temperature and thermal hysteresis width. By analyzing the spatial correlations of the maps in relation to the magnetocrystalline anisotropy and external magnetic field, we detect a reorientation of domain walls across the phase transition. The employed statistical approach can be extended to the study of other magnetic phenomena with NV magnetometry or other sensing techniques.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Simultaneous measurement of the exchange parameter and saturation magnetization using propagating spin waves

The exchange interaction in ferromagnetic ultra thin films is a critical parameter in magnetization-based storage and logic devices, yet the accurate measurement of it remains a challenge. While a variety of approaches are currently used to determine the exchange parameter, each has its limitations, and good agreement among them has not been achieved. To date, neutron scattering, magnetometry, Brillouin light scattering, spin-torque ferromagnetic resonance spectroscopy, and Kerr microscopy have all been used to determine the exchange parameter. Here, we present a method that exploits the wavevector selectivity of Brillouin light scattering to measure the spin wave dispersion in both the backward volume and Damon–Eshbach orientations. The exchange, saturation magnetization, and magnetic thickness are then determined by a simultaneous fit of both dispersion branches with general spin wave theory without any prior knowledge of the thickness of a magnetic “dead layer.” In this study, we demonstrate the strength of this technique for ultrathin metallic films, typical of those commonly used in industrial applications for magnetic random-access memory.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Progress toward picosecond on-chip magnetic memory

Here, we offer a perspective on the prospects of ultrafast spintronics and opto-magnetism as a pathway to high-performance, energy-efficient, and non-volatile embedded memory in digital integrated circuit applications. Conventional spintronic devices, such as spin-transfer-torque magnetic-resistive random-access memory (STT-MRAM) and spin–orbit torque MRAM, are promising due to their non-volatility, energy-efficiency, and high endurance. STT-MRAMs are now entering into the commercial market; however, they are limited in write speed to the nanosecond timescale. Improvement in the write speed of spintronic devices can significantly increase their usefulness as viable alternatives to the existing CMOS-based devices. In this article, we discuss recent studies that advance the field of ultrafast spintronics and opto-magnetism. An optimized ferromagnet–ferrimagnet exchange-coupled magnetic stack, which can serve as the free layer of a magnetic tunnel junction (MTJ), can be optically switched in as fast as ~3 ps. Integration of ultrafast magnetic switching of a similar stack into an MTJ device has enabled electrical readout of the switched state using a relatively larger tunneling magnetoresistance ratio. Purely electronic ultrafast spin–orbit torque induced switching of a ferromagnet has been demonstrated using ~6 ps long charge current pulses. We conclude our Perspective by discussing some of the challenges that remain to be addressed to accelerate ultrafast spintronics technologies toward practical implementation in high-performance digital information processing systems.

42 ENGINEERING↗

DOE OSTI2023

Observation of coherently coupled cation spin dynamics in an insulating ferrimagnetic oxide

Many technologically useful magnetic oxides are ferrimagnetic insulators, which consist of chemically distinct cations. In this work, we examine the spin dynamics of different magnetic cations in ferrimagnetic NiZnAl-ferrite (Ni 0.65 Zn 0.35 Al 0.8 Fe 1.2 O 4 ) under continuous microwave excitation. Specifically, we employ time-resolved x-ray ferromagnetic resonance to separately probe Fe 2+/3+ and Ni 2+ cations on different sublattice sites. Our results show that the precessing cation moments retain a rigid, collinear configuration to within ≈2°. Moreover, the effective spin relaxation is identical to within <10% for all magnetic cations in the ferrite. Thus, we validate the oft-assumed “ferromagnetic-like” dynamics in the resonantly driven ferrimagnetic oxide: the magnetic moments from different cations precess as a coherent, collective magnetization, despite the high contents of nonmagnetic Zn 2+ and Al 3+ diluting the exchange interactions.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2024

Enhanced spin pumping in heterostructures of coupled ferrimagnetic garnets

Spin pumping has significant implications for spintronics, providing a mechanism to manipulate and transport spins for information processing. Understanding and harnessing spin currents through spin pumping is critical for the development of efficient spintronic devices. The use of a magnetic insulator with low damping enhances the signal-to-noise ratio in crucial experiments such as spin-torque ferromagnetic resonance (FMR) and spin pumping. A magnetic insulator coupled with a heavy metal or quantum material offers a more straightforward model system, especially when investigating spin-charge interconversion processes to greater accuracy. This simplicity arises from the absence of unwanted effects caused by conduction electrons unlike in ferromagnetic metals. Here, we investigate the spin pumping in coupled ferrimagnetic (FiM) Y 3 Fe 5 O 12 (YIG)/Tm 3 Fe 5 O 12 (TmIG) bilayers combined with heavy-metal (Pt) using the inverse spin Hall effect. It is observed that magnon transmission occurs at both of the FiMs FMR positions. The enhancement of spin pumping voltage (V sp ) in the FiM garnet heterostructures is observed. The plausible reason might be the interfacial exchange coupling between FiMs. The modulation of V sp is achieved by tuning the bilayer structure. Further, the spin mixing conductance for these coupled systems is found to be ≈ 10 18 m –2 . Furthermore, our findings describe a coupled FiM system for the investigation of magnon coupling providing opportunities for magnonic devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Magnetism and spin dynamics in room-temperature van der Waals magnet Fe 5 GeTe 2

Two-dimensional van der Waals (vdWs) materials have gathered a lot of attention recently. However, the majority of these materials have Curie temperatures that are well below room temperature, making it challenging to incorporate them into device applications. In this work, we synthesized a room-temperature vdW magnetic crystal Fe 5 GeTe 2 with a Curie temperature T c = 332 K, and studied its magnetic properties by vibrating sample magnetometry (VSM) and broadband ferromagnetic resonance (FMR) spectroscopy. The experiments were performed with external magnetic fields applied along the c -axis (H∥ c ) and the ab -plane (H∥ ab ), with temperatures ranging from 300 to 10 K. We have found a sizable Landé g -factor difference between the H∥ c and H∥ ab cases. In both cases, the Landé g -factor values deviated from g = 2. This indicates contribution of orbital angular momentum to the magnetic moment. The FMR measurements reveal that Fe 5 GeTe 2 has a damping constant comparable to Permalloy. With reducing temperature, the linewidth was broadened. Together with the VSM data, our measurements indicate that Fe 5 GeTe 2 transitions from ferromagnetic to ferrimagnetic at lower temperatures. Our experiments highlight key information regarding the magnetic state and spin scattering processes in Fe 5 GeTe 2 , which promote the understanding of magnetism in Fe 5 GeTe 2 , leading to implementations of Fe 5 GeTe 2 based room-temperature spintronic devices.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Tuning 2D magnetism in Fe 3+X GeTe 2 films by element doping

Two-dimensional (2D) ferromagnetic materials have been discovered with tunable magnetism and orbital-driven nodal-line features. Controlling the 2D magnetism in exfoliated nanoflakes via electric/magnetic fields enables a boosted Curie temperature (T C ) or phase transitions. One of the challenges, however, is the realization of high T C 2D magnets that are tunable, robust and suitable for large scale fabrication. Here, we report molecular-beam epitaxy growth of wafer-scale Fe 3+X GeTe 2 films with T C above room temperature. By controlling the Fe composition in Fe 3+X GeTe 2 , a continuously modulated T C in a broad range of 185–320 K has been achieved. This widely tunable T C is attributed to the doped interlayer Fe that provides a 40% enhancement around the optimal composition X = 2. We further fabricated magnetic tunneling junction device arrays that exhibit clear tunneling signals. Our results show an effective and reliable approach, i.e. element doping, to producing robust and tunable ferromagnetism beyond room temperature in a large-scale 2D Fe 3+X GeTe 2 fashion.

2D ferromagnetic material↗

DOE OSTI2021

Enhanced Interface-Driven Perpendicular Magnetic Anisotropy by Symmetry Control in Oxide Superlattices

Perpendicular magnetic anisotropy (PMA) has recently been shown to emerge at interfaces of 3d and 5d transition-metal oxides (TMOs). However, strategies to systematically stabilize such interface-driven PMA still remains elusive, hindering further applications of this design approach. Here, tuning crystal symmetry is shown to be an effective means to engineer this interfacial phenomenon. The evolution of PMA strength as a function of ferromagnetic oxide thickness quantitatively reveals the competition between volume- and interface-specific contributions that determine the magnetic anisotropy. By applying different degrees of epitaxial strain, the relative contributions to PMA are modulated, clearly revealing their correlations with crystal symmetries. To be more specific, the volume anisotropy energy is found to be correlated with the tetragonal distortion of the ferromagnetic layer, while the interface anisotropy energy is mainly modulated by the octahedral tilting at the interface. With these insights, superlattices with enhanced interface-driven PMA and higher Curie temperature are realized. These findings reveal a route to engineering interface-driven PMA and associated magnetic phenomena in TMO heterostructures for future spintronic applications.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Independence of the spin current from the Néel vector orientation in antiferromagnet CoO

Spin pumping from ferromagnetic Fe into antiferromagnetic CoO across a Ag spacer layer was studied using ferromagnetic resonance (FMR) in Py/CoO/Ag/Fe/Ag(001). The thin Py film on top of CoO permits an alignment of the CoO Neél vector through field cooling in two otherwise equivalent [110] and [110] crystalline axes which are parallel and perpendicular to the Fe magnetization direction, respectively. Fe FMR linewidth is measured as a function of Ag thickness in 10-20-GHz frequency range and in 180-330 K temperature range. Furthermore, we find that there exists an anisotropy in the Fe FMR damping for parallel and perpendicular alignment of the Fe and CoO spins. However, such anisotropic damping exists only at thin Ag thickness where there exists a magnetic interlayer coupling between Fe and CoO, and vanishes at thick Ag thickness where the interlayer coupling becomes negligible but permitting spin-current transmission into CoO. Our result indicates the absence of anisotropic spin current for parallel and perpendicular alignment of the Fe and CoO spin axes.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Shortcomings of meta-GGA functionals when describing magnetism

Several recent studies have shown that SCAN, a functional belonging to the meta-generalized gradient approximation (MGGA) family, leads to significantly overestimated magnetic moments in itinerant ferromagnetic metals. However, this behavior is not inherent to the MGGA level of approximation since TPSS, for instance, does not lead to such severe overestimations. In order to provide a broader view of the accuracy of MGGAfunctionals for magnetism, we extend the assessment to more functionals but also to antiferromagnetic solids. The results show that to describe magnetism there is overall no real advantage in using a MGGA functional compared to GGAs. For both types of approximation, an improvement in ferromagnetic metals is necessarily accompanied by a deterioration (underestimation) in antiferromagnetic insulators, and vice versa. Furthermore, we also provide some analysis in order to understand in more detail the relation between the mathematical form of the functionals and the results.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Confined magnons

Magnetic structures are known to possess magnon excitations confined to their surfaces and interfaces, but these spatially localized modes are often not resolved in spectroscopy experiments. In this work, we develop a theory to calculate the confined magnon spectra and its associated spin scattering function, which is the physical observable in neutron and electron scattering, and a proxy for photon spectroscopy based on x-ray, Raman, and terahertz (THz) sources. We show that extra anisotropy at the surface or interface plays a key role in magnon confinement. We obtain analytical expressions for the confinement length scale and show that it is qualitatively similar for ferromagnets and antiferromagnets in dimension d≥2. For d=1, we find remarkable differences between ferromagnetic and antiferromagnetic models. The theory indicates the presence of several confined magnon resonances in addition to the usual magnons thought to explain the excitations of magnetic nanostructures. Detecting these modes may elucidate the impact of the interface on spin anisotropy and magnetic order.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Magnetic damping in ferromagnetic/heavy-metal systems: The role of interfaces and the relation to proximity-induced magnetism

Damping and spin transport in spintronic multilayered systems continues to be a topic of active research. The enhancement of damping in ferromagnet (FM)/spacer layer (SL)/heavy-metal (HM) thin-film systems was studied for Co 25 Fe 75 /SL/Pt with a nonmagnetic (NM) SL of either Au or Cu with variable thickness, in order to understand the correlation with proximity-induced magnetism (PIM) in the HM. Structural, PIM and magnetic damping measurements were undertaken on the same samples. Specifically, secondary ion mass spectroscopy, element specific x-ray magnetic reflectivity and x-ray magnetic circular dichroism at the Pt and Au L 3 edges, and ferromagnetic resonance methods were used. With increasing thickness of a Cu or Au SL directly between the FM and the Pt layer, the Pt PIM and the damping both fall rapidly, with a relationship between damping and PIM that depends on the SL material. The PIM observed in the Au layer showed a complex dependence on the layer thickness, suggesting some hybridization with the Pt. The role of the number and location of interfaces on the damping was demonstrated with the addition of a SL within the Pt layer, which showed that the specific details of the NM/HM interface also affects the damping. The insertion of a Cu SL within the Pt showed a measurable increase in the overall enhancement of the damping while the insertion of a Au SL into Pt had almost no effect on the damping. Finally, together these results demonstrate the role of both PIM and of additional interfaces in the enhancement of damping in FM/HM systems, which is not fully accounted for by existing theory

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Spin-exchange Hamiltonian and topological degeneracies in elemental gadolinium

In this report we present a comprehensive study of the magnetic exchange Hamiltonian of elemental gadolinium. We use neutron scattering to measure the magnon spectrum over the entire Brillouin zone and fit the excitations to a spin wave model to extract the first 26 nearest-neighbor magnetic exchange interactions with rigorously defined uncertainty. We find these exchange interactions to follow RKKY behavior, oscillating from ferromagnetic to antiferromagnetic as a function of distance. Finally, we discuss the topological features and degeneracies in Gd, and HCP ferromagnets in general. We show theoretically how, with asymmetric exchange, topological properties could be tuned with a magnetic field.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Planar Hall Driven Torque in a Ferromagnet/Nonmagnet/Ferromagnet System

An important goal of spintronics is to covert a charge current into a spin current with a controlled spin polarization that can exert torques on an adjacent magnetic layer. Here we demonstrate such torques in a two ferromagnet system. A CoNi multilayer is used as a spin current source in a sample with structure CoNi/Au/CoFeB. Spin torque ferromagnetic resonance is used to measure the torque on the CoFeB layer. The response as a function of the applied field angle and current is consistent with the symmetry expected for a torque produced by the planar Hall effect originating in CoNi. We find the strength of this effect to be comparable to that of the spin Hall effect in platinum, indicating that the planar Hall effect holds potential as a spin current source with a controllable polarization direction.

ferromagnetic resonance↗