Tilted Spins in Chains of Molecular Switches on Pb(100).

A complex based on a Ni(II) porphyrin exhibiting spin crossover on Ag(111) is studied on Pb(100) by scanning tunneling microscopy at 0.3 K. Strong molecular interactions between the phenyl and pentafluorophenyl moieties lead to the formation of molecular chains and cause a faceting of the substrate surface. The chains are located along double and multiple substrate steps that deviate from high-symmetry directions. Tunneling spectroscopy reveals spin-flip excitations of an S = 1 system. Measurements in high magnetic fields are used to identify a tilt of the complex and its hard anisotropy axis with respect to the surface normal. Electron injection into the substrate near the molecular rows induces a transition to a state with larger inelastic cross section, leaving the spin state unchanged.

Magnetic-anisotropy modulation in multiferroic heterostructures by ferroelectric domains from first principles.

First-principles calculations incorporating spin-orbit coupling are presented for a multiferroic material as a ferromagnetic/ferroelectric junction. We simulate the interface effect that cannot be described by the single-phase bulk. The in-plane uniaxial magnetic-anisotropy of Co2FeSi is observed when the ferroelectric domain is polarized parallel to the interface, whereas the magnetic anisotropy is significantly different in the plane for the electrical polarization perpendicular to the interface. While the single-phase effect dominates the main part of the modulation of the magnetic anisotropy, symmetry breaking due to the interfacial effect is observed in the ferromagnetic ultrathin films. The origin of the modulated magnetic-anisotropy can be attributed to the shifting of specific energy bands in Co2FeSi when the ferroelectric domain is modified.

The origin of strain-induced magnetocrystalline anisotropy in multiferroic Co₂FeSi/BaTiO₃(001) heterostructures is clarified by first-principles electron theory. The magnetic anisotropy is modified by interface effects for ultrathin Co₂FeSi films.

Transformation of in-plane to out-of-plane anisotropy in MnBi alloy for permanent magnet application: a First-principles study.

The low-temperature phase (LTP) MnBi exhibits remarkable ferromagnetic properties at room temperature. However, below its Curie temperature ( T C ), a phase transition occurs around 613 K due to diffusion of Mn into interstitial sites, raising concerns about its structural and magnetic properties. Furthermore, the presence of in-plane anisotropy in LTP-MnBi alloy at low temperatures raises concerns about its suitability for use in permanent magnet applications, even at higher temperature. Therefore, this study examines the structural and magnetic properties of pure LTP-MnBi and its successive Ni-doped and Fe-substituted alloys using first-principles study based on density functional theory (DFT). To prevent Mn diffusion into interstitial sites, Ni doping is employed. Additionally, the incorporation of Ni successfully addresses the in-plane anisotropy issue in LTP-MnBi, transforming it into out-of-plane anisotropy. Moreover, we explored the potential advantages of substituting Fe for one of Mn site. This substitution aims to improve the observed dynamical instability in Ni-doped alloy and to further enhanced the magnetocrystalline anisotropy energy (MAE) of the material, resulting in an MAE of 3.21 MJ/m3, along with a T C of 523 K. Therefore, the coexistence of high MAE and moderate T C in the Mn0.5Fe0.5Bi-Ni alloy presents viable option for its application in permanent magnet technology.

An Antiferromagnetic Neuromorphic Memory Based on Perpendicularly Magnetized CoO.

Antiferromagnets (AFMs) are ideal materials to boost neuromorphic computing toward the ultrahigh speed and ultracompact integration regime. However, developing a suitable AFM neuromorphic memory remains an aspirational but challenging goal. In this work, we construct such a memory based on the CoO/Pt heterostructure, in which the collinear insulating AFM CoO shows a strong perpendicular anisotropy facilitating its electrical readout and writing. Utilizing the unique nonlinear response and bipolar fading memory properties of the device, we demonstrate a multidimensional reservoir computing beyond the traditional binary paradigm. These results are expected to pave the way toward next-generation fast and massive neuromorphic computing.

The Role of Rare-Earth Atoms in the Anisotropy and Antiferromagnetic Exchange Coupling at a Hybrid Metal-Organic Interface.

Magnetic anisotropy and magnetic exchange interactions are crucial parameters that characterize the hybrid metal-organic interface, a key component of an organic spintronic device. It is shown that the incorporation of 4f RE atoms to hybrid metal-organic interfaces of CuPc/REAu2 type (RE = Gd, Ho) constitutes a feasible approach toward on-demand magnetic properties and functionalities. The GdAu2 and HoAu2 substrates differ in their magnetic anisotropy behavior. Remarkably, the HoAu2 surface promotes the inherent out-of-plane anisotropy of CuPc, owing to the match between the anisotropy axis of substrate and molecule. Furthermore, the presence of RE atoms leads to a spontaneous antiferromagnetic exchange coupling at the interface, induced by the 3d-4f superexchange interaction between the unpaired 3d electron of CuPc and the 4f electrons of the RE atoms. It is shown that 4f RE atoms with unquenched quantum orbital momentum ( L $L$ ), as it is the case of Ho, induce an anisotropic interfacial exchange coupling.

The Use of External Fields (Magnetic, Electric, and Strain) in Molecular Beam Epitaxy-The Method and Application Examples.

Molecular beam epitaxy (MBE) is a powerful tool in modern technologies, including electronic, optoelectronic, spintronic, and sensoric applications. The primary factor determining epitaxial heterostructure properties is the growth mode and the resulting atomic structure and microstructure. In this paper, we present a novel method for growing epitaxial layers and nanostructures with specific and optimized structural and magnetic properties by assisting the MBE process using electromagnetic and mechanical external stimuli: an electric field (EF), a magnetic field (MF), and a strain field (SF). The transmission of the external fields to the sample is realized using a system of specialized sample holders, advanced transfers, and dedicated manipulators. Examples of applications include the influence of MFs on the growth and anisotropy of epitaxial magnetite and iron films, the use of EFs for in situ resistivity measurements, the realization of in situ magneto-optic measurements, and the application of SFs to the structural modification of metal films on mica.

Control of Anisotropy and Magnetic Hyperthermia Effect by Addition of Cobalt on Magnetite Nanoparticles.

Magnetic hyperthermia (MH) has emerged as a promising technology with diverse applications in medical and technological fields, leveraging the remote induction of temperature elevation through an alternating magnetic field. While Fe3O4 nanoparticles with an average size around 12-25 nm are commonly employed in MH systems, this study introduces a strategy to produce smaller particles (less than or equal to 10 nm) with enhanced heating efficiency, as measured by specific power absorption (SPA). We conducted an exhaustive and detailed investigation into the morphological and magnetic properties of CoxFe3-xO4 nanoparticles, aiming to optimize their MH response. By varying the Co content, we successfully tuned the effective magnetic anisotropy while maintaining saturation magnetization nearly constant. The MH analysis indicates that these nanoparticles predominantly heat through the Néel mechanism, demonstrating robust reproducibility across different concentrations, viscosity mediums, and ac field conditions. Notably, we identified an optimal anisotropy or Co concentration that maximizes SPA, crucial for developing magnetic systems requiring particles with specific sizes. This work contributes to advancing the understanding and application of MH, particularly in tailoring nanoparticle properties for targeted and efficient heat generation in various contexts.

Magnetic irreversibility and magnetization processes in Ni5Al3/NiO core/shell nanoparticle system.

This work brings out many interesting facets of magnetism in the Ni5Al3/NiO core/shell nanoparticle system. Theweakandstrongmagnetic irreversibility lines (TWI(H)andTSI(H)) reproduce the previously reportedH - Tphase diagram at fieldsH⩽30 Oe, but strong departures occur forH > 30 Oe. Comparison with the theoretically predictedH - Tphase diagram allows us to identifyTWIwithTCG+SG, where the paramagnetic (PM)-chiral glass (CG) and PM-spin glass (SG) phase transitions occursimultaneously, andTSIwithTSG, the temperature at which transition to the replica symmetry breakingSGstate takes place. TheTSI(H)transition line abruptly ends at the point (H≃30 Oe,T≃90K). AsHexceeds 30 Oe, a new transition appears which gets completely suppressed at fieldsH>1 kOewhere the magnetic irreversibility ceases to exist. Nointrinsiclong-range ferromagnetic ordering exists but fields as low as 3 kOe suffice to induce long-range ferromagnetic order. At fixed temperatures, the magnetocrystalline anisotropy fluctuations essentially govern the 'approach-to-saturation' in magnetization for fields in the range 3 - 70 kOe. The present nanocrystalline system behaves as an isotropic system with random easy axis in which the magnetization reversal occurs through the coherent rotation of the magnetizations of weakly-interacting single-domain Ni5Al3particles. Saturation magnetization, likeM(T) atH⩾2 kOe, exhibits an anomalous upturn at temperatures below ≈ 30 K. This upturn is associated with the anomalous softening of spin-wave modes which results in the thermal excitation of a large number of non-equilibrium (finite lifetime) magnons. At sub-Kelvin temperatures, these magnons undergo Bose-Einstein condensation.

On the origin of magnetic anisotropy in 4f-free ferromagnets based on the CaCu5structure.

Using first-principles calculations, we investigate the origin of magnetocrystalline anisotropy in a series of 4f-electron-free intermetallics with CaCu5-based structures: YCo5, YCo4B, and Y3Co13B2. The electronic structure of these compounds is characterized by a set of narrow 3dbands near the Fermi level. In YCo5the easy-axis anisotropy originates primarily in the spin-orbit coupling-induced mixing of the electronic states with Codx2-y2anddxycharacter. The analysis ofk-resolved anisotropy shows that positive contributions accumulate from the entire Brillouin zone but are particularly large near thekz=0plane. The analysis of the single-site and two-site terms reveals a large positive single-site contribution to the magnetocrystalline anisotropy from the Co atoms on the honeycomb sublattice, along with two-site contributions from both honeycomb and kagome sublattices.

Spin-wave dynamics in perpendicularly magnetized antidot multilayers.

Using all-optical time-resolved magneto-optical Kerr effect measurements we demonstrate an efficient modulation of the spin-wave (SW) dynamics via the bias magnetic field orientation around nanoscale diamond shaped antidots that are arranged on a square lattice within a [Co(0.75 nm)/Pd(0.9 nm)]8multilayer with perpendicular magnetic anisotropy (PMA). Micromagnetic modeling of the experimental results reveals that the SW modes in the lower frequency regime are related to narrow shell regions around the antidots, where in-plane (IP) domain structures are formed due to the reduced PMA, caused by Ga+ion irradiation during the focused ion beam milling process of antidot fabrication. The IP direction of the shell magnetization undergoes a striking change with magnetic field orientation, leading to the sharp variation of the edge localized (shell) SW modes. Nevertheless, the coupling between such edge localized and bulk SWs for different orientations of bias field in PMA systems gives rise to interesting Physics and attests to new prospects for developing energy efficient and hybrid-system-based next-generation nanoscale magnonic devices.

Enhanced Ferromagnetism and Tunable Magnetic Anisotropy in a van der Waals Ferromagnet.

2D van der Waals (vdW) magnets have recently emerged as a promising material system for spintronic device innovations due to their intriguing phenomena in the reduced dimension and simple integration of magnetic heterostructures without the restriction of lattice matching. However, it is still challenging to realize Curie temperature far above room temperature and controllable magnetic anisotropy for spintronics application in 2D vdW magnetic materials. In this work, the pressure-tuned dome-like ferromagnetic-paramagnetic phase diagram in an iron-based 2D layered ferromagnet Fe3GaTe2 is reported. Continuously tunable magnetic anisotropy from out-of-plane to in-plane direction is achieved via the application of pressure. Such behavior is attributed to the competition between intralayer and interlayer exchange interactions and enhanced DOS near the Fermi level. The study presents the prominent properties of pressure-engineered 2D ferromagnetic materials, which can be used in the next-generation spintronic devices.

Elevating the Performance of Heterometallic 3d/4f SMMs: The Role of Diamagnetic CoIII and ZnII Ions in Magnetization Dynamics.

Recent advances in the synthesis of 3d/4f Single-Molecule Magnets (SMMs) have revealed the effective role of incorporating diamagnetic CoIII or ZnII ions to enhance the magnetic properties of LnIII ions. This concept highlights notable examples of CoIII/LnIII and ZnII/LnIII SMMs documented in the recent literature, illustrating how the selection of various peripheral and/or bridging ligands can modulate the magnetic anisotropy of 4f metal ions, thereby increasing their energy barriers.

Levamisole Based Co(II) Single-Ion Magnet.

A new Co(II) complex, [Co(NCS)2(L)2] (1) has been synthesized based on levamisole (L) as a new ligand. Single-crystal X-ray diffraction analyses confirm that the Co(II) ion is having a distorted tetrahedral coordination geometry in the complex. Notably strong intramolecular S⋅⋅⋅S and S⋅⋅⋅N interactions has been confirmed by employing Quantum Theory of Atoms in Molecules (QTAIM). These intramolecular interactions occur among the sulfur and nitrogen atoms of the levamisole ligands and also the nitrogen atoms of the thiocyanate. Direct current (dc) magnetic analyses reveal presence of zero field splitting (ZFS) and large magnetic anisotropy on Co(II). Detailed ab initio ligand field theory calculations quantitatively predicted the magnitude of ZFS. Prominent field-induced single-ion magnet (SIM) behavior was observed for 1 from dynamic magnetization measurements. Slow magnetic relaxation follows an Orbach mechanism with the effective energy barrier Ueff=29.6 (7) K and relaxation time τo=1.4 (4)×10-9 s.

Field-Free Manipulation of Two-Dimensional Ferromagnet CrTe2 by Spin-Orbit Torques.

Electrical manipulation of magnetic states in two-dimensional ferromagnetic systems is crucial in information storage and low-dimensional spintronics. Spin-orbit torque presents a rapid and energy-efficient method for electrical control of the magnetization. In this letter, we demonstrate a wafer-scale spin-orbit torque switching of two-dimensional ferromagnetic states. Using molecular beam epitaxy, we fabricate two-dimensional heterostructures composed of low crystal-symmetry WTe2 and ferromagnet CrTe2 with perpendicular anisotropy. By utilizing out-of-plane spins generated from WTe2, we achieve field-free switching of the CrTe2 perpendicular magnetization. The threshold switching current density in CrTe2/WTe2 is 1.2 × 106 A/cm2, 20 times smaller than that of the CrTe2/Pt control sample even with an external magnetic field. In addition, the switching behavior can be modulated by external magnetic fields and crystal symmetry. Our findings demonstrate a controllable and all-electric manipulation of perpendicular magnetization in a two-dimensional ferromagnet, representing a significant advancement toward the practical implementation of low-dimensional spintronic devices.

Theoretical Study of Microwires with an Inhomogeneous Magnetic Structure Using Magnetoimpedance Tomography.

The recently proposed magnetoimpedance tomography method is based on the analysis of the frequency dependences of the impedance measured at different external magnetic fields. The method allows one to analyze the distribution of magnetic properties over the cross-section of the ferromagnetic conductor. Here, we describe the example of theoretical study of the magnetoimpedance effect in an amorphous microwire with inhomogeneous magnetic structure. In the framework of the proposed model, it is assumed that the microwire cross-section consists of several regions with different features of the effective anisotropy. The distribution of the electromagnetic fields and the microwire impedance are found by an analytical solution of Maxwell equations in the particular regions. The field and frequency dependences of the microwire impedance are analyzed taking into account the frequency dependence of the permeability values in the considered regions. Although the calculations are given for the case of amorphous microwires, the obtained results can be useful for the development of the magnetoimpedance tomography method adaptation for different types of ferromagnetic conductors.

Dimensionality Engineering of Magnetic Anisotropy from the Anomalous Hall Effect in Synthetic SrRuO3 Crystals.

Magnetic anisotropy in atomically thin correlated heterostructures is essential for exploring quantum magnetic phases for next-generation spintronics. Whereas previous studies have mostly focused on van der Waals systems, here we investigate the impact of dimensionality of epitaxially grown correlated oxides down to the monolayer limit on structural, magnetic, and orbital anisotropies. By designing oxide superlattices with a correlated ferromagnetic SrRuO3 and nonmagnetic SrTiO3 layers, we observed modulated ferromagnetic behavior with the change of the SrRuO3 thickness. Especially, for three-unit-cell-thick layers, we observe a significant 1500% improvement of the coercive field in the anomalous Hall effect, which cannot be solely attributed to the dimensional crossover in ferromagnetism. The atomic-scale heterostructures further reveal the systematic modulation of anisotropy for the lattice structure and orbital hybridization, explaining the enhanced magnetic anisotropy. Our findings provide valuable insights into engineering the anisotropic hybridization of synthetic magnetic crystals, offering a tunable spin order for various applications.

Unusual Dzyaloshinskii-Moriya Interaction in Graphene/Fe3GeTe2 Van der Waals Heterostructure.

Dzyaloshinskii-Moriya interaction (DMI) is shown to induce a topologically protected chiral spin texture in magnetic/nonmagnetic heterostructures. In the context of van der Waals spintronic devices, graphene emerges as an excellent candidate material. However, due to its negligible spin-orbit interaction, inducing DMI to stabilize topological spins when coupled to 3d-ferromagnets remains challenging. Here, it is demonstrated that, despite these challenges, a sizeable Rashba-type spin splitting followed by significant DMI is induced in graphene/Fe3GeTe2. This is made possible due to an interfacial electric field driven by charge asymmetry together with the broken inversion symmetry of the heterostructure. These findings reveal that the enhanced DMI energy parameter, resulting from a large effective electron mass in Fe3GeTe2, remarkably contributes to stabilizing non-collinear spins below the Curie temperature, overcoming the magnetic anisotropy energy. These results are supported by the topological Hall effect, which coexists with the non-trivial breakdown of Fermi liquid behavior, confirming the interplay between spins and non-trivial topology. This work paves the way toward the design and control of interface-driven skyrmion-based devices.

Single-Phase L10-Ordered High Entropy Thin Films with High Magnetic Anisotropy.

The vast high entropy alloy (HEA) composition space is promising for discovery of new material phases with unique properties. This study explores the potential to achieve rare-earth-free high magnetic anisotropy materials in single-phase HEA thin films. Thin films of FeCoNiMnCu sputtered on thermally oxidized Si/SiO2 substrates at room temperature are magnetically soft, with a coercivity on the order of 10 Oe. After post-deposition rapid thermal annealing (RTA), the films exhibit a single face-centered-cubic phase, with an almost 40-fold increase in coercivity. Inclusion of 50 at.% Pt in the film leads to ordering of a single L10 high entropy intermetallic phase after RTA, along with high magnetic anisotropy and 3 orders of magnitude coercivity increase. These results demonstrate a promising HEA approach to achieve high magnetic anisotropy materials using RTA.

Six-Coordinated CoII Single-Molecule Magnets: Synthetic Strategy, Structure and Magnetic Properties.

The pursuit of molecule-based magnetic memory materials contributes significantly to high-density information storage research in the frame of the ongoing information technologies revolution. Remarkable progress has been achieved in both transition metal (TM) and lanthanide based single-molecule magnets (SMMs). Notably, six-coordinated CoII SMMs hold particular research significance owing to the economic and abundant nature of 3d TM ions compared to lanthanide ions, the substantial spin-orbit coupling of CoII ions, the potential for precise control over coordination geometry, and the air-stability of coordination-saturated structures. In this review, we will summarize the progress made in six-coordinated CoII SMMs, organized by their coordination geometry and molecular structure similarity. Valuable insights, principles, and new mechanism gleaned from this research and remaining issues that need to be addressed will also be discussed to guide future optimization.

Temperature Induced Reversible Switching of the Magnetic Anisotropy in a Neodymium Complex Adsorbed on Graphite.

Controlling the magnetic anisotropy of molecular layers assembled on a surface is one of the challenges that needs to be addressed to create the next-generation spintronic devices. Recently, metal complexes that show a reversible solid-state switch of their magnetic anisotropy in response to physical stimuli, such as temperature and magnetic field, have been discovered. The complex Nd(trensal) (H3trensal = 2,2',2''-tris(salicylideneimino)triethylamine) is predicted to exhibit such property. An ultra-thin film of Nd(trensal) is deposited on highly ordered pyrolytic graphite as a proof-of-concept system to show that this property can be retained at the nanoscale on a layered material. By combining single crystal magnetometric measurements and synchrotron X-ray-based absorption techniques, supported by multiplet ligand field simulations based on the trigonal crystal field surrounding the lanthanide centre, it is demonstrated that changing the temperature reverses the magnetic anisotropy of an ordered film of Nd(trensal), thus opening significant perspectives for the realization of a novel family of temperature-controlled molecular spintronic devices.