Generation Spintronic Devices Research Articles

Centimeter-scale above room temperature ferromagnetic Fe3GaTe2 thin films by molecular beam epitaxy

Abstract Fe3GaTe2, as a layered ferromagnetic material, has a Curie temperature (T c ) higher than room temperature, making it the key material in the next generation of spintronic devices. To be used in practical devices, large-size and high-quality Fe3GaTe2 thin films need to be prepared. Here, the centimeter-scale thin film samples with high crystal quality and above room temperature ferromagnetism with strong perpendicular magnetic anisotropy (PMA) have been prepared by molecular beam epitaxy technology. Furthermore, the T c of the samples raises as the film thickness increases, and reaches 367 K when the film thickness is 60 nm. This study provides material foundations for the new generation of van der Waals spintronic devices and paves the way for the commercial application of Fe3GaTe2.

Chiral π-Conjugated Double Helical Aminyl Diradical with the Triplet Ground State

We describe effective development of the highly diastereoselective synthesis of double helical tetraamine 2-H2-C2 and propose a mechanism for its formation. The resolution of 2-H2-C2 is facilitated by a high racemization barrier of 43 kcal mol-1 and it is implemented via either a chiral auxiliary or preparative supercritical fluid chromatography. This enables preparation of the first high-spin neutral diradical, with spin density delocalized within an enantiomeric double helical π-system. The presence of two effective 3-electron C–N bonds in the diradical leads to: (1) the triplet (S = 1) high-spin ground state with a singlet-triplet energy gap of 0.4 kcal mol-1 and (2) the long half-life of up to 6 days in 2-MeTHF at room temperature. The diradical possesses a racemization barrier of at least 26 kcal mol-1 in 2-MeTHF at 293 K and chiroptical properties, with absorption anisotropy factor |g| ≈ 0.005 at 548 nm. These unique magnetic and optical properties of our diradical form the basis for the development of next generation spintronic devices.

Boosting the Curie temperature of GaN monolayer through van der Waals heterostructures

The pursuit of van der Waals (vdW) heterostructures with high Curie temperature and strong perpendicular magnetic anisotropy (PMA) is vital to the advancement of next generation spintronic devices. First-principles calculations are used to study the electronic structures and magnetic characteristics of GaN/VS2 vdW heterostructure under biaxial strain and electrostatic doping. Our findings show that a ferromagnetic ground state with a remarkable Curie temperature (477 K), much above room temperature, exists in GaN/VS2 vdW heterostructure and 100% spin polarization efficiency. Additionally, GaN/VS2 vdW heterostructure still maintains PMA under biaxial strain, which is indispensable for high-density information storage. We further explore the electron, magnetic, and transport properties of VS2/GaN/VS2 vdW sandwich heterostructure, where the magnetoresistivity can reach as high as 40%. Our research indicates that the heterostructure constructed by combining the ferromagnet VS2 and the non-magnetic semiconductor GaN is a promising material for vdW spin valve devices at room temperature.

Stoichiometry-Tunable Synthesis and Magnetic Property Exploration of Two-Dimensional Chromium Selenides.

Emerging 2D chromium-based dichalcogenides (CrXn (X = S, Se, Te; 0 < n ≤ 2)) have provoked enormous interests due to their abundant structures, intriguing electronic and magnetic properties, excellent environmental stability, and great application potentials in next generation electronics and spintronics devices. Achieving stoichiometry-controlled synthesis of 2D CrXn is of paramount significance for such envisioned investigations. Herein, we report the stoichiometry-controlled syntheses of 2D chromium selenide (CrxSey) materials (rhombohedral Cr2Se3 and monoclinic Cr3Se4) via a Cr-self-intercalation route by designing two typical chemical vapor deposition (CVD) strategies. We have also clarified the different growth mechanisms, distinct chemical compositions, and crystal structures of the two type materials. Intriguingly, we reveal that the ultrathin Cr2Se3 nanosheets exhibit a metallic feature, while the Cr3Se4 nanosheets present a transition from p-type semiconductor to metal upon increasing the flake thickness. Moreover, we have also uncovered the ferromagnetic properties of 2D Cr2Se3 and Cr3Se4 below ∼70 K and ∼270 K, respectively. Briefly, this research should promote the stoichiometric-ratio controllable syntheses of 2D magnetic materials, and the property explorations toward next generation spintronics and magneto-optoelectronics related applications.

A Novel Ferroelectric Rashba Semiconductor.

Fast, reversible, and low-power manipulation of the spin texture is crucial for next generation spintronic devices like non-volatile bipolar memories, switchable spin current injectors or spin field effect transistors. Ferroelectric Rashba semiconductors (FERSC) are the ideal class of materials for the realization of such devices. Their ferroelectric character enables an electronic control of the Rashba-type spin texture by means of the reversible and switchable polarization. Yet, only very few materials are established to belong to this class of multifunctional materials. Here, Pb1- xGexTe is unraveled as a novel FERSC system down to nanoscale. The ferroelectric phase transition and concomitant lattice distortion are demonstrated by temperature dependent X-ray diffraction, and their effect on electronic properties are measured by angle-resolved photoemission spectroscopy. In few nanometer-thick epitaxial heterostructures, a large Rashba spin-splitting is exhibiting a wide tuning range as a function of temperature and Ge content. This work defines Pb1- xGexTe as a high-potential FERSC system for spintronic applications.

Highly Efficient Spin-Orbit Torque Switching in Bi2Se3/Fe3GeTe2 van der Waals Heterostructures.

Topological insulators (TIs) have shown promise as a spin-generating layer to switch the magnetization state of ferromagnets via spin-orbit torque (SOT) due to charge-to-spin conversion efficiency of the TI surface states that arises from spin-momentum locking. However, when TIs are interfaced with conventional bulk ferromagnetic metals, the combination of charge transfer and hybridization can potentially destroy the spin texture and hamper the possibility of accessing the TI surface states. Here, we fabricate an all van der Waals (vdW) heterostructure consisting of molecular beam epitaxy grown bulk-insulating Bi2Se3 and exfoliated 2D metallic ferromagnet Fe3GeTe2 (FGT) with perpendicular anisotropy. By detecting the magnetization state of the FGT via anomalous Hall effect and magneto-optical Kerr effect measurements, we determine the critical switching current density for magnetization switching to be Jc ≈ 1.2 × 106 A/cm2, the lowest reported for the switching of a perpendicular anisotropy ferromagnet using Bi2Se3. From second harmonic Hall measurements, we further determine the SOT efficiency (ξDL) to be in the range of 1.8 ± 0.3 and 1.4 ± 0.08 between 5 and 150 K, comparable to the highest values reported for Bi2Se3. Our density functional theory calculations find that the weak interlayer interactions at the Bi2Se3/FGT interface lead to a weakened dipole at the interface and suppress the proximity induced magnetic moment on Bi2Se3. This enables direct access to the TI surface states contributed by the first quintuple layer, where the spins are singly degenerate with significant net in-plane spin polarization. Our results highlight the clear advantage of all-vdW heterostructures with weak interlayer interactions that can enhance SOT efficiency and minimize critical current density, an important step toward realizing next generation low-power nonvolatile memory and spintronic devices.

From Solution to Surface: Persistence of the Diradical Character of a Diindenoanthracene Derivative on a Metallic Substrate.

Organic diradicals are envisioned as elementary building blocks for designing a new generation of spintronic devices and have been used in constructing prototypical field effect transistors and nonlinear optical devices. Open-shell systems, however, are also reactive, thus requiring design strategies to "protect" their radical character from the environment, especially when they are embedded in solid-state devices. Here, we report the persistence on a metallic surface of the diradical character of a diindeno[b,i]anthracene (DIAn) core protected by bulky end-groups. Our scanning tunneling spectroscopy measurements on single-molecules detected singlet-triplet excitations that were absent for DIAn species packed in assembled structures. Density functional theory simulations unravel that the molecular geometry on the metal substrate can crucially modify the value of the singlet-triplet gap via the delocalization of the radical sites. The persistence of the diradical character over metallic substrates is a promising finding for integrating radical-based materials into functional devices.

Identifying Rashba–Dresselhaus splittings from first-principle calculations: A brief overview

The present review is aimed to understand the Rashba and Dresselhaus effects from the first-principle calculations. A brief overview of first-principle density functional theory (DFT) and its global acceptance have been discussed. The discussions of the Rashba–Dresselhaus splittings, spin textures and understanding the effects from first-principle DFT calculations have been highlighted. Rashba and Dresselhaus effects have gained much attention in recent era for their highly promising applications in spintronics. In the presence of spin-orbit coupling and inherent non-centrosymmetry, while BiTeCl, TiS2Se, rhombohedral CsPbF3 and BiCoO3 compounds show large values of Rashba parameter ([Formula: see text] of [Formula: see text], 1.10, 1.05 and 0.74[Formula: see text]eVÅ, respectively, the single-layered semiconductor nanostructure InSb, rhombohedral BiFeO3 and Ag2BiO3 systems however depict promising values of Dresselhaus parameter ([Formula: see text] of [Formula: see text], 0.50 and 0.15[Formula: see text]eVÅ, respectively. The future of Rashba–Dresselhaus effects and their advancements in spintronics have also been enlightened in this paper. We believe that this study will not only help to understand the Rashba–Dresselhaus effects from first-principle calculations, but can also augment their applications in next generation spintronic devices.

Light-Induced Metastable Hidden Skyrmion Phase in the Mott Insulator Cu2 OSeO3.

The discovery of a novel long-lived metastable skyrmion phase in the multiferroic insulator Cu2 OSeO3 visualized with Lorentz transmission electron microscopy for magnetic fields below the equilibrium skyrmion pocket is reported. This phase can be accessed by exciting the sample non-adiabatically with near-infrared femtosecond laser pulses and cannot be reached by any conventional field-cooling protocol, referred as a hidden phase. From the strong wavelength dependence of the photocreation process and via spin-dynamics simulations, the magnetoelastic effect is identified as the most likely photocreation mechanism. This effect results in a transient modification of the magnetic free energy landscape extending the equilibrium skyrmion pocket to lower magnetic fields. The evolution of the photoinduced phase is monitored for over 15 min and no decay is found. Because such a time is much longer than the duration of any transient effect induced by a laser pulse in a material, it is assumed that the newly discovered skyrmion state is stable for practical purposes, thus breaking ground for a novel approach to control magnetic state on demand at ultrafast timescales and drastically reducing heat dissipation relevant for next-generation spintronicdevices.

Reversible conversion between skyrmions and skyrmioniums

Skyrmions and skyrmioniums are topologically non-trivial spin textures found in chiral magnetic systems. Understanding the dynamics of these particle-like excitations is crucial for leveraging their diverse functionalities in spintronic devices. This study investigates the dynamics and evolution of chiral spin textures in [Pt/Co]3/Ru/[Co/Pt]3 multilayers with ferromagnetic interlayer exchange coupling. By precisely controlling the excitation and relaxation processes through combined magnetic field and electric current manipulation, reversible conversion between skyrmions and skyrmioniums is achieved. Additionally, we observe the topological conversion from a skyrmionium to a skyrmion, characterized by the sudden emergence of the skyrmion Hall effect. The experimental realization of reversible conversion between distinct magnetic topological spin textures represents a significant development that promises to expedite the advancement of the next generation of spintronic devices.

Correlation of Interface Interdiffusion and Skyrmionic Phases.

Magnetic skyrmions are prime candidates for the next generation of spintronic devices. Skyrmions and other topological magnetic structures are known to be stabilized by the Dzyaloshinskii-Moriya interaction (DMI) that occurs when the inversion symmetry is broken in thin films. Here, we show by first-principles calculations and atomistic spin dynamics simulations that metastable skyrmionic states can also be found in nominally symmetric multilayered systems. We demonstrate that this is correlated with the large enhancement of the DMI strength due to the presence of local defects. In particular, we find that metastable skyrmions can occur in Pd/Co/Pd multilayers without external magnetic fields and can be stable even near room temperature conditions. Our theoretical findings corroborate with magnetic force microscopy images and X-ray magnetic circular dichroism measurements and highlight the possibility of tuning the intensity of DMI by using interdiffusion at thin film interfaces.

Magneto-strain effects in 2D ferromagnetic van der Waal material CrGeTe_3

The idea of strain based manipulation of spins in magnetic two-dimensional (2D) van der Waal (vdW) materials leads to the development of new generation spintronic devices. Magneto-strain arises in these materials due to the thermal fluctuations and magnetic interactions which influences both the lattice dynamics and the electronic bands. Here, we report the mechanism of magneto-strain effects in a vdW material CrGeTe_3 across the ferromagnetic (FM) transition. We find an isostructural transition in CrGeTe_3 across the FM ordering with first order type lattice modulation. Larger in-plane lattice contraction than out-of-plane give rise to magnetocrystalline anisotropy. The signature of magneto-strain effects in the electronic structure are shift of the bands away from the Fermi level, band broadening and the twinned bands in the FM phase. We find that the in-plane lattice contraction increases the on-site Coulomb correlation (U_{eff}) between Cr atoms resulting in the band shift. Out-of-plane lattice contraction enhances the d-p hybridization between Cr–Ge and Cr–Te atoms which lead to band broadening and strong spin-orbit coupling (SOC) in FM phase. The interplay between U_{eff} and SOC out-of-plane gives rise to the twinned bands associated with the interlayer interactions while the in-plane interactions gives rise to the 2D spin polarized states in the FM phase.

Mirroring Skyrmions in Synthetic Antiferromagnets via Modular Design.

Skyrmions are promising for the next generation of spintronic devices, which involves the production and transfer of skyrmions. The creation of skyrmions can be realized by a magnetic field, electric field, or electric current while the controllable transfer of skyrmions is hindered by the skyrmion Hall effect. Here, we propose utilizing the interlayer exchange coupling induced by the Ruderman-Kittel-Kasuya-Yoshida interactions to create skyrmions through hybrid ferromagnet/synthetic antiferromagnet structures. An initial skyrmion in ferromagnetic regions could create a mirroring skyrmion with an opposite topological charge in antiferromagnetic regions driven by the current. Furthermore, the created skyrmions could be transferred in synthetic antiferromagnets without deviations away from the main trajectories due to the suppression of the skyrmion Hall effect in comparison to the transfer of the skyrmion in ferromagnets. The interlayer exchange coupling can be tuned, and the mirrored skyrmions can be separated when they reach the desired locations. Using this approach, the antiferromagnetic coupled skyrmions can be repeatedly created in hybrid ferromagnet/synthetic antiferromagnet structures. Our work not only supplies a highly efficient approach to create isolated skyrmions and correct the errors in the process of skyrmion transport, but also paves the way to a vital information writing technique based on the motion of skyrmions for skyrmion-based data storage and logic devices.

Non-uniform superlattice magnetic tunnel junctions

We propose a new class of non-uniform superlattice magnetic tunnel junctions (Nu-SLTJs) with the linear, Gaussian, Lorentzian, and Pöschl–Teller width and height based profiles manifesting a sizable enhancement in the TMR (≈104 − 106%) with a significant suppression in the switching bias (≈9 folds) owing to the physics of broad-band spin filtering. By exploring the negative differential resistance region in the current–voltage characteristics of the various Nu-SLTJs, we predict the Nu-SLTJs offer fastest spin transfer torque switching in the order of a few hundred picoseconds. We self-consistently employ the atomistic non-equilibrium Green’s function formalism coupled with the Landau–Lifshitz–Gilbert–Slonczewski equation to evaluate the device performance of the various Nu-SLTJs. We also present the design of minimal three-barrier Nu-SLTJs having significant TMR (≈104%) and large spin current for the ease of device fabrication. We hope that the class of Nu-SLTJs proposed in this work may lay the bedrock to embark on the exhilarating voyage of exploring various non-uniform superlattices for the next generation of spintronic devices.

Driving skyrmions with low threshold current density in Pt/CoFeB thin film

Magnetic skyrmions are topologically stable spin swirling particle like entities which are appealing for next generation spintronic devices. The expected low critical current density for the motion of skyrmions makes them potential candidates for future energy efficient electronic devices. Several heavy metal/ferromagnetic (HM/FM) systems have been explored in the past decade to achieve faster skyrmion velocity at low current densities. In this context, we have studied Pt/CoFeB/MgO heterostructures in which skyrmions have been stabilized at room temperature (RT). It has been observed that the shape of the skyrmions are perturbed even by the small stray field arising from low moment magnetic tips while performing the magnetic force microscopy (MFM), indicating presence of low pinning landscape in the samples. This hypothesis is indeed confirmed by the low threshold current density to drive the skyrmions in our sample, at velocities of few ∼10 m s−1.

Strain- and thickness-dependent magnetic properties of epitaxial La0.67Sr0.33CoO3/La0.67Sr0.33MnO3 bilayers

Magnetic properties and interfacial phenomena of epitaxial perovskite oxides depend sensitively on parameters such as film thickness and strain state. In this work, epitaxial La0.67Sr0.33CoO3 (LSCO)/La0.67Sr0.33MnO3 (LSMO) bilayers were grown on NdGaO3 (NGO) and LaAlO3 (LAO) substrates with a fixed LSMO thickness of 6 nm, and LSCO thickness (tLSCO) varying from 2 to 10 nm. Soft x-ray magnetic spectroscopy revealed that magnetically active Co2+ ions that strongly coupled to the LSMO layer were observed below a critical tLSCO for bilayers grown on both substrates. On LAO substrates, this critical thickness was 2 nm, above which the formation of Co2+ ions was quickly suppressed leaving only a soft LSCO layer with mixed valence Co3+/Co4+ ions. The magnetic properties of both LSCO and LSMO layers displayed strong tLSCO dependence. This critical tLSCO increased to 4 nm on NGO substrates, and the magnetic properties of only the LSCO layer displayed tLSCO dependence. A non-magnetic layer characterized by Co3+ ions and with a thickness below 2 nm exists at the LSCO/substrate interface for both substrates. The results contribute to the understanding of interfacial exchange spring behavior needed for applications in next generation spintronic and magnetic memory devices.

TM2B3 monolayers: Intrinsic anti-ferromagnetism and Dirac nodal line semimetal

Searching for two-dimensional materials combining both magnetic order and topological order is of great significance for quantum devices and spintronic devices. Here, a class of two-dimensional transition metal borides, TM2B3 (TM = Ti–Ni), with high stability and stable antiferromagnetic (AFM) orders was predicted by using the first-principles method. The result shows that they possess large magnetic anisotropy energy and high critical temperature. Interestingly, Mn2B3 monolayer is confirmed to be AFM Dirac node line semimetal with several Dirac points near the Fermi level. Detailed analysis of the irreducible representations shows that the nodal lines are protected by the horizontal mirror symmetry Mz. Our findings provide an excellent platform for exploring topological and magnetic materials ready for the next generation of spintronic devices.

Optimizing the quality of epitaxial Y3Fe5O12 thin films via a two-step post-annealing process

Background: Yttrium iron garnet (Y3Fe5O12, YIG) is a prototype magnetic garnet, which possesses the lowest magnetic damping (α) value so far on the earth among all discovered or synthesized materials. This makes it the best candidate for categories of next generation spintronic devices, possessing great application potentials. Methods: A two-step annealing method, with first annealing carried out at a relative low temperature and second annealing at a relatively higher temperature, had been used for the first time to crystallize room temperature sputtered amorphous Y3Fe5O12 (YIG) films on Gd3Ga5O12 (GGG) substrates. The crystalline structure, surface morphology, static and dynamic magnetic properties of the obtained YIG films were characterized through X-ray diffraction (XRD), atomic force microscopy (AFM), vibrating sample magnetometer (VSM) and ferromagnetic resonance (FMR) systems, respectively. Results: It was found that the YIG films obtained via this elaborate annealing method, have a much smoother surface, lower coercivity field, and better dynamic magnetic properties, than that of the YIG films annealed by ordinary one-step approach. Particularly, the ferromagnetic resonance (FMR) linewidth of the best two-step annealed 25 nm YIG film is lower than ~7 Oe at frequency of 10 GHz. Conclusions: Our work clarifies that this two-step annealing approach can effectively improve the quality of the obtained epitaxial YIG films on GGG substrates.

Noncollinear magnetism in two-dimensional CrTe2

The discovery of two-dimensional (2D) van der Waals magnets opened unprecedented opportunities for the fundamental exploration of magnetism in quantum materials and the realization of next generation spintronic devices. Here, based on a multiscale modelling approach that combines first-principles calculations and a Heisenberg model supplied with ab-initio parameters, we report a strong magnetoelastic coupling in a free-standing monolayer of CrTe2. We demonstrate that different crystal structures of a single CrTe2 give rise to non-collinear magnetism through magnetic frustration and emergence of the Dzyaloshinskii–Moriya interaction. Utilizing atomistic spin dynamics, we perform a detailed investigation of the complex magnetic properties pertaining to this 2D material impacted by the presence of various types of structural distortions akin to charge density waves.

Enhancement of Exchange Bias and Perpendicular Magnetic Anisotropy in CoO/Co Multilayer Thin Films by Tuning the Alumina Template Nanohole Size.

The interest in magnetic nanostructures exhibiting perpendicular magnetic anisotropy and exchange bias (EB) effect has increased in recent years owing to their applications in a new generation of spintronic devices that combine several functionalities. We present a nanofabrication process used to induce a significant out-of-plane component of the magnetic easy axis and EB. In this study, 30 nm thick CoO/Co multilayers were deposited on nanostructured alumina templates with a broad range of pore diameters, 34 nm ≤ Dp ≤ 96 nm, maintaining the hexagonal lattice parameter at 107 nm. Increase of the exchange bias field (HEB) and the coercivity (HC) (12 times and 27 times, respectively) was observed in the nanostructured films compared to the non-patterned film. The marked dependence of HEB and HC with antidot hole diameters pinpoints an in-plane to out-of-plane changeover of the magnetic anisotropy at a nanohole diameter of ∼75 nm. Micromagnetic simulation shows the existence of antiferromagnetic layers that generate an exceptional magnetic configuration around the holes, named as antivortex-state. This configuration induces extra high-energy superdomain walls for edge-to-edge distance >27 nm and high-energy stripe magnetic domains below 27 nm, which could play an important role in the change of the magnetic easy axis towards the perpendicular direction.