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DOE OSTI2024

Epitaxial Growth of Large-Scale 2D CrTe 2 Films on Amorphous Silicon Wafers With Low Thermal Budget

2D van der Waals (vdW) magnets open landmark horizons in the development of innovative spintronic device architectures. However, their fabrication with large scale poses challenges due to high synthesis temperatures (>500 °C) and difficulties in integrating them with standard complementary metal-oxide semiconductor (CMOS) technology on amorphous substrates such as silicon oxide (SiO 2 ) and silicon nitride (SiN x ). Here, a seeded growth technique for crystallizing CrTe 2 films on amorphous SiN x /Si and SiO 2 /Si substrates with a low thermal budget is presented. This fabrication process optimizes large-scale, granular atomic layers on amorphous substrates, yielding a substantial coercivity of 11.5 kilo-oersted, attributed to weak intergranular exchange coupling. Field-driven Néel-type stripe domain dynamics explain the amplified coercivity. Moreover, the granular CrTe 2 devices on Si wafers display significantly enhanced magnetoresistance, more than doubling that of single-crystalline counterparts. Current-assisted magnetization switching, enabled by a substantial spin–orbit torque with a large spin Hall angle (85) and spin Hall conductivity (1.02 × 10 7 ℏ/2e Ω -1 m -1 ), is also demonstrated. These observations underscore the proficiency in manipulating crystallinity within integrated 2D magnetic films on Si wafers, paving the way for large-scale batch manufacturing of practical magnetoelectronic and spintronic devices, heralding a new era of technological innovation.

2D magnetic thin films↗

DOE OSTI2022

Evidence for spin swapping in an antiferromagnet

Antiferromagnetic insulators offer strategic advantages in spintronic applications because of their negligible stray fields and ultrafast magnetic dynamics. Control of their magnetization and readout of their magnetic state are essential for these applications but remain challenging. In this work, we report the electrical detection of room-temperature magnetization switching in the canted antiferromagnetic insulator LaFeO 3 , capped with a Pt or W overlayer. The observation of a large magneto-thermovoltage with an in-plane temperature gradient suggests that the mechanism is the swapping of spin currents in the antiferromagnet. This effect provides a sensitive electrical probe of the tiny net magnetization in the insulator, which can be manipulated by a magnetic field on the order of 10 mT. Our results highlight a new material class of insulating canted antiferromagnets for spintronics and spin caloritronics and suggests a method for the electrical readout of magnetic signals in an antiferromagnetic insulator. Electrical readout of the state of an antiferromagnet is an important goal for spintronic applications. Now, detection of the electrical voltage created by a thermal gradient in a canted antiferromagnet suggests a route for achieving this goal.

42 ENGINEERING↗

DOE OSTI2021

Interposed pulsed power system for fast separation of radioactive beams

This paper presents the novel design of an interposed pulsed power system, developed to drive a fast-switching magnet with a large multi-mH load inductance, and high field amplitude (> 1 T). This modulator can produce variable flat-top pulses from 1 to 30 ms with rise and fall times of less than 0.5 ms at a variable duty cycle of 3–91% into a heavily inductive load. The system employs a novel over-voltage topology to overcome the inherent inductance and achieve the fast rise and fall times, switching to a precision DC supply to efficiently maintain the flattop without requiring many-kV voltage. We present a power source design consideration, including the results of computer modeling as well as the first experimental results of a modulator scaled test model will also be presented.

47 OTHER INSTRUMENTATION↗

DOE OSTI2022

Quantum Sensing and Imaging of Spin–Orbit-Torque-Driven Spin Dynamics in the Non-Collinear Antiferromagnet Mn 3 Sn

Novel non-collinear antiferromagnets with spontaneous time-reversal symmetry breaking, non-trivial band topology, and unconventional transport properties have received immense research interest over the past decade due to their rich physics and enormous promise in technological applications. One of the central focuses in this emerging field is exploring the relationship between the microscopic magnetic structure and exotic material properties. Nanoscale imaging of both spin–orbit-torque-induced deterministic magnetic switching and chiral spin rotation in non-collinear antiferromagnet Mn 3 Sn films using nitrogen-vacancy (NV) centers are reported. Direct evidence of the off-resonance dipole–dipole coupling between the spin dynamics in Mn 3 Sn and proximate NV centers is also demonstrated by NV relaxometry measurements. These results demonstrate the unique capabilities of NV centers in accessing the local information of the magnetic order and dynamics in these emergent quantum materials and suggest new opportunities for investigating the interplay between topology and magnetism in a broad range of topological magnets.

36 MATERIALS SCIENCE↗

DOE OSTI2022

ZrTe2/CrTe2: an epitaxial van der Waals platform for spintronics

Abstract The rapid discovery of two-dimensional (2D) van der Waals (vdW) quantum materials has led to heterostructures that integrate diverse quantum functionalities such as topological phases, magnetism, and superconductivity. In this context, the epitaxial synthesis of vdW heterostructures with well-controlled interfaces is an attractive route towards wafer-scale platforms for systematically exploring fundamental properties and fashioning proof-of-concept devices. Here, we use molecular beam epitaxy to synthesize a vdW heterostructure that interfaces two material systems of contemporary interest: a 2D ferromagnet (1T-CrTe 2 ) and a topological semimetal (ZrTe 2 ). We find that one unit-cell (u.c.) thick 1T-CrTe 2 grown epitaxially on ZrTe 2 is a 2D ferromagnet with a clear anomalous Hall effect. In thicker samples (12 u.c. thick CrTe 2 ), the anomalous Hall effect has characteristics that may arise from real-space Berry curvature. Finally, in ultrathin CrTe 2 (3 u.c. thickness), we demonstrate current-driven magnetization switching in a full vdW topological semimetal/2D ferromagnet heterostructure device.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Highly Efficient Room‐Temperature Spin‐Orbit‐Torque Switching in a Van der Waals Heterostructure of Topological Insulator and Ferromagnet

Abstract All‐Van der Waals (vdW)‐material‐based heterostructures with atomically sharp interfaces offer a versatile platform for high‐performing spintronic functionalities at room temperature. One of the key components is vdW topological insulators (TIs), which can produce a strong spin‐orbit‐torque (SOT) through the spin‐momentum locking of their topological surface state (TSS). However, the relatively low conductance of the TSS introduces a current leakage problem through the bulk states of the TI or the adjacent ferromagnetic metal layers, reducing the interfacial charge‐to‐spin conversion efficiency ( q ICS ). Here, a vdW heterostructure is used consisting of atomically‐thin layers of a bulk‐insulating TI Sn‐doped Bi 1.1 Sb 0.9 Te 2 S 1 and a room‐temperature ferromagnet Fe 3 GaTe 2, to enhance the relative current ratio on the TSS up to ≈20%. The resulting q ICS reaches ≈1.65 nm −1 and the critical current density J c ≈0.9 × 10 6 Acm −2 at 300 K, surpassing the performance of TI‐based and heavy‐metal‐based SOT devices. These findings demonstrate that an all‐vdW heterostructure with thickness optimization offers a promising platform for efficient current‐controlled magnetization switching at room temperature.

2D ferromagnet↗

DOE OSTI2023

Strength distributions of laminated FeNi-based metal amorphous nanocomposite ribbons

Metal Amorphous Nanocomposite (MANC) materials offer low losses at high magnetic switching frequency, enabling high power density motors with increased rotational speed. While MANCs have high strength, they are brittle. The use of motor components such as a rotor consisting of brittle material presents a reliability concern. Here, a promising MANC alloy is subjected to tensile tests and failure is observed with high-speed photography. A method is developed to prepare tensile specimens of laminated MANC and epoxy layers, simulating the stacking of an epoxy-impregnated tape-wound core. Tensile tests are conducted for single layer ribbon and for five- and ten-layer stacks of laminated material with thin layers of thermosetting epoxy. Failure distributions are shown to have increasing Weibull modulus with increasing layer count. The composite MANC material system is modeled using chain-of-bundles models. Using a k-failure model, we show that single ribbon strength distribution data can be used to predict well the failure distribution of laminated stacks. The agreement occurs when the assumed ineffective length, over which load is recovered in a failed layer, is comparable to the observed interlaminar separation length.

24 POWER TRANSMISSION AND DISTRIBUTION↗

DOE OSTI2022

Tuning Spin-Orbit Torques Across the Phase Transition in VO 2 /NiFe Heterostructure

The emergence of spin-orbit torques as a promising approach to energy-efficient magnetic switching has generated large interest in material systems with easily and fully tunable spin-orbit torques. We report current-induced spin-orbit torques in VO 2 /NiFe heterostructures are investigated using spin-torque ferromagnetic resonance, where the VO 2 layer undergoes a prominent insulator-metal transition. A roughly twofold increase in the Gilbert damping parameter, α, with temperature is attributed to the change in the VO 2 /NiFe interface spin absorption across the VO 2 phase transition. More remarkably, a large modulation (±100%) and a sign change of the current-induced spin-orbit torque across the VO 2 phase transition suggest two competing spin-orbit torque generating mechanisms. The bulk spin Hall effect in metallic VO 2 , corroborated by the first-principles calculation of the spin Hall conductivity σ SH ≈ -10 4 ($\frac{\hbar}{e}$) Ω -1 m -1 , is verified as the main source of the spin-orbit torque in the metallic phase. The self-induced/anomalous torque in NiFe, with opposite sign and a similar magnitude to the bulk spin Hall effect in metallic VO 2 , can be the other competing mechanism that dominates as temperature decreases. For applications, the strong tunability of the torque strength and direction opens a new route to tailor spin-orbit torques of materials that undergo phase transitions for new device functionalities.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Understanding and Tuning the Electronic Properties of Prussian Blue Analogues

Prussian blue analogues (PBAs) have attracted increasing interest owing to their potential applications in various fields such as energy storage and conversion, neuromorphic computing, and magnetic switching. With a general formula of A x M N [M C (CN) 6 ], they feature an open framework that provides abundant channels for diffusion of alkali metal ions A and allows flexible compositional control of transition metal ions M N and M C . The oxidation states of transition metal ions can be tuned by adjusting the amount (x) of alkali ions A. Here, we carried out density functional theory calculations combined with experimental measurements to investigate the effects of transition metal ions, alkali ions, and oxidation states on the electronic properties of PBAs. Our calculations found that the band gaps of PBAs can be tuned from close to 0 eV to more than 4 eV. Experimentally, we introduced the synthesis/characterization of five previously unreported PBAs (M N = Ru, Os; M C = Fe, Ru, and Os) to complete the nine stable M N :M C transition metal combinations in group VIII of the periodic table. The optically measured intervalence charge transfer excitation energies of group VIII PBAs are consistent with calculated band gaps. They demonstrate wide band gap tunability by adjusting transition metals and oxidation states, enabling semiconductor-to-metal transitions for memristor applications and enhancing electronic conductivity for battery applications. In conclusion, this work provides a computational/experimental database of electronic properties versus structural compositions for PBAs.

Electrical conductivity↗

DOE OSTI2024

Terahertz electric-field-driven dynamical multiferroicity in SrTiO 3

The emergence of collective order in matter is among the most fundamental and intriguing phenomena in physics. In recent years, the dynamical control and creation of novel ordered states of matter not accessible in thermodynamic equilibrium is receiving much attention. The theoretical concept of dynamical multiferroicity has been introduced to describe the emergence of magnetization due to time-dependent electric polarization in non-ferromagnetic materials. In simple terms, the coherent rotating motion of the ions in a crystal induces a magnetic moment along the axis of rotation. Here we provide experimental evidence of room-temperature magnetization in the archetypal paraelectric perovskite SrTiO 3 due to this mechanism. We resonantly drive the infrared-active soft phonon mode with an intense circularly polarized terahertz electric field and detect the time-resolved magneto-optical Kerr effect. A simple model, which includes two coupled nonlinear oscillators whose forces and couplings are derived with ab initio calculations using self-consistent phonon theory at a finite temperature, reproduces qualitatively our experimental observations. A quantitatively correct magnitude was obtained for the effect by also considering the phonon analogue of the reciprocal of the Einstein–de Haas effect, which is also called the Barnett effect, in which the total angular momentum from the phonon order is transferred to the electronic one. Our findings show a new path for the control of magnetism, for example, for ultrafast magnetic switches, by coherently controlling the lattice vibrations with light.

36 MATERIALS SCIENCE↗

DOE OSTI2023

A feasible path for the use of ferromagnetic josephson junctions in quantum circuits: The ferro-transmon

We discuss the capabilities of ferromagnetic (F) Josephson junctions (JJs) in a variety of layouts and configurations. The main goal is to demonstrate the potential of these hybrid JJs to disclose new physics and the possibility to integrate them in superconducting classical and quantum electronics for various applications. The feasible path towards the use of ferromagnetic Josephson junctions in quantum circuits starts from experiments demonstrating macroscopic quantum tunneling in NbN/GdN/NbN junctions with ferro-insulator barriers and with triplet components of the supercurrent, supported by a self-consistent electrodynamic characterization as a function of the barrier thickness. This has inspired further studies on tunnel ferromagnetic junctions with a different layout and promoted the first generation of ferromagnetic Al-based JJs, specifically Al/AlO x /Al/Py/Al. This layout takes advantage of the capability to integrate the ferromagnetic layer in the junction without affecting the quality of the superconducting electrodes and of the tunnel barrier. The high quality of the devices paves the way for the possible implementation of Al tunnel-ferromagnetic JJs in superconducting quantum circuits. These achievements have promoted the notion of a novel type of qubit incorporating ferromagnetic JJs. This qubit is based on a transmon design featuring a tunnel JJ in parallel with a ferromagnetic JJ inside a SQUID loop capacitively coupled to a superconducting readout resonator. In conclusion, the effect of an external RF field on the magnetic switching processes of ferromagnetic JJs has been also investigated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2026

Critical structural parameter determining magnetic phases in the F⁡e 2 ⁢M⁢o 3 ⁢O 8 altermagnet system

A systematic structural investigation of F⁡e 2 ⁢M⁢o 3⁢ O 8 as a function of pressure, temperature, and magnetic field reveals that the 𝑃⁢6 3 ⁢𝑚⁢𝑐 space group remains robust over a wide range of conditions. No changes in the long-range crystal structure are observed for pressures up to 10 GPa, temperatures between 11 K and 300 K, and magnetic fields up to 9 T. The magnetostructural response, quantified by Δ⁢𝑐/𝑐, is determined for magnetic fields applied transverse to the crystallographic 𝑐 axis, demonstrating strong magnetoelastic coupling. The well-known magnetic-field-induced transition is confirmed to be first order and isostructural, occurring between two distinct altermagnetic states. Importantly, this transition can also be accessed using magnetic fields applied within the 𝑎𝑏 plane. When expressed in terms of the 𝑐/𝑎 ratio, the structural evolution under pressure (0–10 GPa) maps continuously onto that observed across the full Zn substitution range in (F⁡e 1−𝑦⁢ Z⁢n 𝑦 )2 M⁢o 3 ⁢O 8 ⁢(0 ≤ 𝑦 ≤ 1), indicating a common underlying structural control parameter. Furthermore, these results demonstrate that the 𝑐-axis lattice parameter is the primary structural degree of freedom governing magnetic behavior under external tuning parameters. More broadly, they indicate that magnetic order in this family of complex oxides (𝐴 2 ⁢M⁢o 3 ⁢O 8 , 𝐴 = Co,Mn,Ni) can be systematically tuned via pressure. This tunability highlights these materials as promising platforms for controllable magnetic switching, particularly in thin films integrated with piezoelectric substrates.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Half-Metal Spin Filter for Highly Polarized Emission from GaAs Photocathodes

GaAs-based photocathodes are one of the major sources of spin-polarized electrons and are crucial for the upcoming Electron-Ion collider experiments which includes study of proton spin and spin parity violation in the standard model. The theoretical polarization limit in unstrained GaAs photocathodes is 50 % but only 35 % is routinely achieved in experiments. Spin selective filtering allows to boost the spin polarization beyond the 50 % theoretical limit. In this work, first-principle electronic calculations using standard Density Functional Theory are performed to predict possible Heusler alloy half-metal candidates to be used as spin-filter. Simulations are also performed to investigate the half-metallicity as function of the magnetic spin direction. Several devices are experimentally fabricated using dedicated Molecular Beam Epitaxy growth system. We implemented Quantum Efficiency and Polarization testing of these half-metal/GaAs heterostructures using a dedicated Mott polarimeter system. Photoemission can also be seen on magnetically switching the spin-filter direction accompanied by a change in sign of the asymmetry which is a qualitative proof of the spin-filtering effect.

Poddar, S.↗

DOE OSTI2024

Frequency-independent optical spin injection in Weyl semimetals

We demonstrate that in Weyl semimetals, the momentum-space helical spin texture can couple to the chirality of the Weyl node to generate a frequency-independent optical spin injection. This frequency-independence is rooted in the topology of the Weyl node. Since the helicity and the chirality are always locked for Weyl nodes, the injected spin from a pair of Weyl nodes always add up, implying no symmetry requirements for Weyl semimetals. Finally, we show that such frequency-independent spin injection is robust against multiband corrections and lattice-regularization effect and capable of realizing all-optical magnetization switching in the THz regime.

Gao, Yang↗

DOE OSTI2023

IMS Rapid Response 2023-2 (RR 2023-RND-2): Magnetic order in layered bismuthide RhMnBi 3 (Final Report)

Microelectronics are technologies (mostly theoretical at this point) to create electronic circuits with components of atomic length scale. One of the key materials innovations enabling this technology is exfoliatable two-dimensional materials. These materials allow thin sheets of only a few atoms thick to be easily created in the laboratory. More and more of these materials are reported every year, but few have been characterized in detail. Thus a major goal in materials research in pursuit of microelectronic devices is characterizing newly discovered materials to evaluate their properties. The goal of this project was the measure and understand the magnetic order in a newly discovered van der Waals magnet RhMnBi 3 . Bulk property experiments indicated very complicated magnetic behavior, with multiple phase transitions between 2K and 300K (room temperature). This potentially indicated highly sensitive and tunable magnetism appropriate for single-layer magnetic switches and sensors.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Topological Surface and Bulk States in Dirac Semimetal Alpha-Sn Thin Films

Supported by this DOE grant, we made significant advancements in the study and application of topological surface states (TSS) in topological Dirac semimetal (TDS) α-Sn thin films. Our key findings include: (1) the successful growth of TDS α-Sn thin films via sputtering, an industry-friendly technique, on Si and InSb substrates, marking a breakthrough over previous molecular beam epitaxy methods, (2) the demonstration of enhanced damping in adjacent NiFe thin films due to the TSS of α-Sn, (3) the first observation of a strong bilinear magneto-electric resistance (BMER) effect in TDS materials at room temperature, with responses surpassing previous results, (4) the identification of quantum oscillations in α-Sn thin films associated with the TSS, revealing critical quantum transport characteristics such as Berry phase and quantum mobility, (5) the first experimental observation of negative magnetoresistance in α-Sn, and (6) the demonstration of spinorbit torque-driven, field-free magnetization switching in an α-Sn/Ag/CoFeB trilayer, achieving efficiency levels higher than conventional heavy-metal-based structures, highlighting the essential role of TSS in enabling the switching process.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Integrated transmission electron microscope

An integrated transmission electron microscope comprising multiple electron sources for tuned beams of ultrafast, scanning probe, and parallel illumination in varied beam energies can be alternated within sub-microseconds onto a sample with dynamic ‘transient state’ processes to acquire atomic-scale structural/chemical data with site specificity. The various electron sources and condenser optics enable high-resolution imaging, high-temporal resolution imaging, and chemical imaging, using fast-switching magnets to direct the different electron beams onto a single maneuverable objective pole piece where the sample resides. Such multimodal in situ characterization tools housed in a single microscope have the potential to revolutionize materials science.

Jungjohann, Katherine L.↗

DOE OSTI2020

Giant Magnetoelectric Coupling and Magnetic-Field-Induced Permanent Switching in a Spin Crossover Mn(III) Complex

We investigate giant magnetoelectric coupling at a Mn 3+ spin crossover in [Mn III L]BPh 4 (L = (3,5-diBr-sal) 2 323) with a field-induced permanent switching of the structural, electric, and magnetic properties. An applied magnetic field induces a first-order phase transition from a high spin/low spin (HS-LS) ordered phase to a HS-only phase at 87.5 K that remains after the field is removed. We observe this unusual effect for DC magnetic fields as low as 8.7 T. The spin-state switching driven by the magnetic field in the bistable molecular material is accompanied by a change in electric polarization amplitude and direction due to a symmetry-breaking phase transition between polar space groups. The magnetoelectric coupling occurs due to a γη 2 coupling between the order parameter γ related to the spin-state bistability and the symmetry-breaking order parameter η responsible for the change of symmetry between polar structural phases. We also observe conductivity occurring during the spin crossover and evaluate the possibility that it results from conducting phase boundaries. We perform ab initio calculations to understand the origin of the electric polarization change as well as the conductivity during the spin crossover. Thus, in this work, we demonstrate a giant magnetoelectric effect with a field-induced electric polarization change that is 1/10 of the record for any material.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗