Abstract Phase transition materials such as NdNiO 3 (NNO) when coupled with low damping ferromagnets such as La 0.67 Sr 0.33 MnO 3 (LSMO) hold the promise for developing new multi-functional material systems harnessing the interplay of charge, spin, and orbital degrees of freedom. In this study, we probe the evolution of spin-to-charge conversion in epitaxial all-oxide LSMO (12 nm)/NNO (4, 8, and 16 nm) bilayers. Using spin pumping ferromagnetic resonance, we track the spin-to-charge conversion within the NNO layer through the paramagnetic metal to antiferromagnetic insulator transition and observe a pronounced enhancement of the inverse spin Hall effect signal at the onset of this phase transition. We attribute this enhancement to the electronic and magnetic disorder in NNO at the first-order phase transition, thereby providing insights into the mechanism of spin transport through the phase transition. The tunability of spin-to-charge conversion in this low damping bilayer system offers a pathway for developing reconfigurable, energy-efficient spintronic devices.
Memory effects arise in many complex systems, from protein folding, to the spreading of epidemics and financial decisions. While so-called non-Markovian dynamics is common in larger systems with interacting components, observations in fundamental physical systems have been confined to specifically engineered cases. Here, we report the experimental observation of non-Markovian dynamics in an elemental material, crystalline cobalt. By driving this material with an intense terahertz electromagnetic field, we bring its magnetisation into a non-equilibrium state and follow its evolution. We measure the sample's low temperature magnetic response in the time domain which leads to an unexpectedly rich multi-peaked spectrum in the Fourier domain, that cannot be explained by established models. We use open quantum system theory, which predicts a non-Markovian memory kernel in the dynamical equations to capture the fundamental interaction between the spin system and the phonon bath. Simulations based on this theory produce a multi-peaked spectrum, which matches the measured one. Our non-Markovian approach is also able to reproduce the modification of the spectrum at higher temperatures. Our findings demonstrate that non-Markovian effects are observable at a much more fundamental level than previously thought, opening the door to their exploration and control in a broad range of condensed matter systems.
The Fe/Gd multilayer system hosts a number of magnetic phases, such as stripe, mixed stripe and skyrmion, skyrmion lattice, and isolated skyrmions for a wide range of temperature and magnetic field. We report different Hall transport signals in a Fe/Gd system through multimodal correlative resonant soft x-ray scattering (RSXS), Hall effect, magneto-optic Kerr effect, and transmission x-ray microscopy measurements. The simultaneous nature of the RSXS and Hall transport measurements allowed us to accurately connect various features in the transport data with the specific magnetic phases. We found that the topological Hall effect (THE) shows peaks with opposite signs, which we attribute to two different mechanisms. Our multimodal correlative study indicates that the sign reversal in THE occurs when the system transforms to and from a skyrmion lattice and low density isolated skyrmion phases. We propose that the skyrmion lattice contributes to the THE through a Berry phase induced emergent magnetic field mechanism in one case, and a skew scattering mechanism corresponding to the isolated low density skyrmion state.
Spin-orbit torques have emerged as a powerful mechanism for manipulating magnetic moments in spintronic devices, offering a pathway to more efficient and scalable memory and logic technologies. While conventional spin-orbit torques generated in heavy metals and topological insulators have been extensively studied, recent advancements in unconventional spin-orbit torques demonstrated out-of-plane spin polarizations that could effectively switch perpendicular magnetizations without the need for additional external in-plane magnetic fields, promising significant implications for the development of energy-efficient and compact spintronic devices. Unconventional spin-orbit torques are usually found in materials with low symmetries, such as transition metal dichalcogenides, topological insulators, and 2-D materials. Here, we provide a brief overview of unconventional spin-orbit torques and present two example material systems: CrPt3 and MoTe2, both exhibiting strong spin-orbit coupling and phase-dependent spin-orbit torques, and focus on their unique origins and potential applications. We discuss the roles of magnetic and crystallographic orders in generating unconventional spin-orbit torques, highlighting how these factors contribute to the observed anisotropic and directional dependencies.
The rapid rise of AI has exposed significant limitations in conventional Von Neumann computing architecture, particularly in regard to speed and energy efficiency. To address these challenges, researchers are exploring a brain-inspired neuromorphic architecture that mimics biological neural networks, enabling massive parallel processing with reduced power consumption for complex AI computational demands. Recent interest has focused on utilizing battery electrodes and solid electrolyte materials for their resistive switching properties in developing a neuromorphic architecture. These properties are precisely tuned through local- and bulk-level chemical composition modifications via voltage bias stimuli. In this study, we demonstrate fabricating a three-terminal lithium-ion electrochemical transistor based on lithium titanium oxide (Li4Ti5O12), a popular lithium-ion battery anode material. We deposited and characterized LTO thin films using RF sputtering, demonstrating a 6 orders of magnitude increase in electronic conductivity upon lithiation, with conductivity plateauing after 20% lithiation. Density functional theory calculations revealed transformation from the insulating to conducting state, supported by experimental characterization through X-Ray Photoelectron Spectroscopy (XPS) and Direct Current (DC) polarization analyses. The fabricated transistor consisted of LTO as the channel layer, gold as source/drain terminals, lithium phosphorus oxynitride (LiPON) as the lithium-ion conductor, and copper as the gate terminal. The device exhibited clear hysteresis in transfer characteristics due to lithium insertion/extraction processes. Long-term potentiation (LTP) and long-term depression (LTD) measurements showed an asymmetric ratio of 1.425 and maximum/minimum conductance ratio of 7.83. When implemented in a deep neural network (DNN) for MNIST handwritten digit recognition, the device achieved 92.03% accuracy over 20 training epochs. Detailed transport mechanism analysis revealed the crucial role of oxygen vacancies and interface effects in device operation. Our preliminary findings establish LTO-based lithium-ion electrochemical transistors as promising candidates for energy-efficient neuromorphic computing applications, offering potential solutions to traditional Von Neumann architecture limitations.
Phase transition materials such as NdNiO3 (NNO) when coupled with low damping ferromagnets such as La_0.67Sr_0.33MnO_3 (LSMO) can lead to new multi-functional material systems harnessing the interplay of charge, spin and orbital degrees of freedom. In this study, we probe the evolution of the spin-to-charge conversion in epitaxial all-oxide LSMO (12 nm)/NNO (4, 8, and 16 nm) bilayers. Using spin pumping ferromagnetic resonance we track the spin-charge conversion in the NNO layer through the paramagnetic metal to antiferromagnetic insulator transition and observe a pronounced enhancement of the inverse spin Hall effect signal at the onset of this transition. We attribute this enhancement to the electronic and magnetic disorder in NNO at the first-order phase transition, thereby providing insights into the mechanism of spin transport through the phase transition. The tunability of spin charge conversion in this low damping bilayer system offers a pathway for developing multifunctional, energy-efficient spintronic devices.
Complex ferromagnetic oxides such as La 0.67 Sr 0.33 MnO 3 (LSMO) offer pathways for creating energy‐efficient spintronic devices with new functionalities. LSMO exhibits high‐temperature ferromagnetism, half metallicity, sharp resonance linewidth, low damping, and a large anisotropic magnetoresistance response. Combined with Pt, a proven material with high spin‐charge conversion efficiency, LSMO can be used to create robust nano‐oscillators for neuromorphic computing. Ferromagnetic resonance (FMR) and device‐level spin‐pumping FMR measurements are performed to investigate the magnetization dynamics and spin transport in NdGaO 3 (110)/LSMO(15 nm)/Pt(0 and 5 nm) thin films ranging from 300 K to 90 K and compare the device performance with Py(7 nm)/Pt(5 nm) sample. The spin current pumped into Pt is quantified to determine the temperature‐dependent influence of interfacial interactions. The generated spin current in the micro‐device is maximum at 170 K for the optimally grown LSMO/Pt films. Additionally, this bilayer system exhibits low magnetic Gilbert damping (0.002), small linewidth (12 Oe), and a large spin Hall angle (≈3.2%) at 170 K. Ex situ deposited LSMO/Pt bilayers demonstrate excellent dynamic response, exhibiting fourfold enhancement in signal output, eightfold reduction in damping, and a threefold reduction in linewidth as compared to the Pt/Py system. Such robust device‐level performance can pave way for energy‐efficient spintronic‐based devices.
Time-resolved ultrafast extreme ultraviolet (EUV) magnetic scattering is used to study laser-driven ultrafast magnetization dynamics of labyrinthine domains in a [Co/Ni/Pt] multilayer. Our measurements at the Co and Ni M-edges reveal distinct ultrafast distortions of the scattering pattern position and width for Ni compared to Co. Ni shows a strong modification of the scattering pattern, 9 to 41 times stronger than Co. As distortions of the labyrinthine pattern in reciprocal space relate to the modification of domain textures in real space, significant differences in Co and Ni highlight a 3D distortion of the domain pattern in the far-from-equilibrium regime.
This study investigates the effects of annealing on the magnetic and structural properties of Co/Pd multilayers, which are promising candidates for perpendicular magnetic tunnel junctions, critical to magneto-resistive random-access memory (MRAM) applications. Co/Pd multilayers with various bilayer counts (5, 10, 15, and 20) were synthesized via DC magnetron sputtering and subjected to annealing at temperatures ranging from 250 to 450 °C. Magnetic measurements, including standard magnetization-vs-field major hysteresis loops and first-order reversal curve analysis, showed that annealing increased coercivity, reaching a maximum of 5100 Oe at 450 °C for 20 bilayers. Magneto-Optical Kerr Effect imaging confirmed domain-wall motion as the switching mechanism, except in the highest temperature annealed samples, which appear to behave more like independent particles. Structural characterization using x-ray diffraction revealed enhanced crystallinity with annealing, indicating improved atomic ordering. Atomic force microscopy demonstrated increased surface roughness with bilayer count due to increased thickness. These results show that Co/Pd-based multilayers are tolerant of high-temperature processing, as required for CMOS-based MRAM.
In 1975 Edwards and Anderson introduced a new paradigm that interacting quenched systems, such as a spin-glass, have a phase transition in which long time memory of spatial patterns is realized without spatial correlations. We show here that the information about the time-dependent correlations above the spin-glass transition are embedded in the four spin correlations of the intensity of speckle pattern. This encodes the spin-orientation memory and can be measured by the technique of resonant magnetic x-ray photon correlation spectroscopy (RM- XPCS). We have implemented this method to observe and accurately characterize the critical slowing down of the spin orientation fluctuations in the classic metallic spin glass alloy Cu_1-xMn_x over time scales of 2 sec. to 2 × 10^4 secs. Remarkably the divergence of the correlation time as a function of temperature is consistent with the Vogel-Vulcher law, universally used to characterize the viscous relaxation time in structural glasses. Our method also opens the way for studying phase transitions in systems such as spin ices, quantum spin liquids, the structural glass transition, as well as possibly provide new perspectives on the multifarious problems in which spin-glass concepts have found applications.
We report the first demonstration of tightly focused femtosecond (fs) circularly polarized Bessel-Gauss beams for wavelength-scale magnetization switching in Pt/Co films. When compared to traditional Gaussian beams, these beams show better focusing and energy efficiency. © 2024 The Author(s)
Spin-orbit torques have emerged as a powerful mechanism for manipulating magnetic moments in spintronic devices, offering a pathway to more efficient and scalable memory and logic technologies. While conventional spin-orbit torques generated in heavy metals and topological insulators have been extensively studied, recent advancements in unconventional spin-orbit torques demonstrated out-of-plane spin polarizations that could effectively switch perpendicular magnetizations without the need for additional external in-plane magnetic fields, promising significant implications for the development of energy-efficient and compact spintronic devices. Unconventional spin-orbit torques are usually found in materials with low symmetries, such as transition metal dichalcogenides, topological insulators, and two-dimensional (2D) materials. Here we provide a brief overview of unconventional spin-orbit torques and present two example material systems: CrPt3 and MoTe2, both exhibiting strong spin-orbit coupling and phase-dependent spin-orbit torques, and focus on their unique origins and potential applications. We discuss the roles of magnetic and crystallographic orders in generating unconventional spin-orbit torques, highlighting how these factors contribute to the observed anisotropic and directional dependencies.
Speckle patterns manifesting from the interaction of coherent X-rays with matter offer a glimpse into the dynamics of nanoscale domains that underpin many emergent phenomena in quantum materials. While the dynamics of the average structure can be followed with time-resolved X-ray diffraction, the ultrafast evolution of local structures in nonequilibrium conditions have thus far eluded detection due to experimental limitations, such as insufficient X-ray coherent flux. Here we demonstrate a nonequilibrium speckle visibility experiment using a split-and-delay setup at an X-ray free-electron laser. Photoinduced electronic domain fluctuations of the magnetic model material Fe_3O_4 reveal changes of the trimeron network configuration due to charge dynamics that exhibit liquid-like fluctuations, analogous to a supercooled liquid phase. This suggests that ultrafast dynamics of electronic heterogeneities under optical stimuli are fundamentally different from thermally-driven ones.
(Received 2023; August 2024; accepted September 2024; published 2024) The topological semimetal CrPt3 has potential for generating unconventional spin torques due to its ferrimagnetic ordering, topological band structure, and high anomalous Hall effect. CrPt3 exhibits ferrimagnetic behavior only in its chemically ordered phase and is paramagnetic in its chemically disordered phase. By controlling the growth and annealing temperatures, we prepare epitaxial films of both chemically ordered and chemically disordered phases of CrPt3, allowing us to investigate the effect of magnetic ordering on unconventional-torque generation. We use angle-dependent spin-torque-ferromagnetic-resonance and second-harmonic Hall measurements to probe the spin torques generated from epitaxial CrPt3 in CrPt3/Cu/Ni81Fe19 heterostructures. With current applied along specific directions with respect to the crystal order, we reveal unconventional spin torques in both ordered and disordered films. When current flows parallel to the [111] and [111] directions, we observe an unconventional fieldlike torque that is opposite in sign for the two directions. Our calculations reveal that this unconventional torque originates from an indirect nonlocal spin-orbit torque due to spin scattering at the CrPt3/Cu interface, in addition to symmetry breaking at this interface.
We report on the role of light's angular momentum in magnetic all-optical switching (AOS), which entails magnetization reversal resulting from ultrafast laser pulses applied to a magnetic structure. The magnetic system is comprised of a ferromagnetic thin film of Co/Pt, excited by femtosecond vortex beams of light carrying spin, orbital angular momentum, or a superposition of both. We find that AOS is predominantly driven by the spin angular momentum of light. The experimental findings suggest that the magnitude of topological charge and handedness of the orbital angular momentum of light do not play a significant role. These results improve our understanding of the basic interactions between magnetism and light, paving the way for further investigation and the creation of all-optical magnetic switching technologies.
The topological semimetal CrPt_3 has potential for generating unconventional spin torques due to its ferrimagnetic ordering, topological band structure, and high anomalous Hall effect. CrPt_3 exhibits ferrimagnetic behavior only in its chemically ordered phase and is paramagnetic in its chemically disordered phase. By controlling the growth and annealing temperatures, epitaxial films of both chemically ordered and disordered phases of CrPt_3 are prepared allowing us to investigate the role of magnetic ordering on unconventional torque generation. We use angle dependent spin-torque ferromagnetic resonance and second harmonic Hall measurements to probe the spin torques generated from epitaxial CrPt_3 in CrPt_3/Cu/Ni_81Fe_19 heterostructures. With current applied along specific directions with respect to the crystal order we reveal unconventional spin torques in both ordered and disordered films. When current flows parallel to the [111] and [111] directions we observe an unconventional field-like torque that is opposite in sign for the two directions. Our calculations reveal that this unconventional torque originates from an indirect nonlocal spin-orbit torque due to spin scattering at the CrPt_3/Cu interface, in addition to symmetry breaking at this interface.
To address the ever‐increasing need for higher speed and density of information storage, recent developments in ultrafast optical switching have focused on deterministic control of magnetic properties of materials using femtosecond circularly polarized optical pulses. However, a monolithic high‐speed optical helicity‐dependent switching at room temperature has remained elusive. In recent years, ultra‐thin flat optical structures, known as metasurfaces, have been developed that offer a versatile way to manipulate electromagnetic fields using subwavelength spatial resolution. Here, a monolithic multilayer nanostructure capable of achieving optical helicity‐dependent switching in arbitrary geometries using femtosecond meta‐circularly polarized optical pulses is theoretically described and experimentally demonstrated at room temperature. The proposed monolithic meta‐magnetic platform provides a practical route to reform the current data memory, storage, and information processing technologies in integrated opto‐magnetic systems, holding great promise for cutting‐edge applications in information, spintronics, sensing, and memory storage devices.