Towards MnN as a replacement for IrMn.

There is an urgent need to identify new antiferromagnetic materials that offer a replacement for IrMn alloys for room temperature and above applications. This is driven by the scarcity and high cost of Ir. Recently, MnN with {002} texture grown on a Ta seed layer has been proposed as a cost-effective alternative. However, two key issues need to be addressed before this material can be considered a realistic alternative to IrMn: thick layers of approximately 30 nm are required due to its relatively low magnetocrystalline anisotropy and nitrogen diffusion into the Ta layer at relatively low temperatures results in poor temperature performance. In this work, we show a potential pathway to overcome these issues. By using a W rather than a Ta seed layer, N diffusion is minimized, if not eliminated, at temperatures exceeding 300 ∘ C . Furthermore, preferential {111} growth is achieved and a significantly enhanced anisotropy, 2.6 · 10 6 erg / cm 3 , has been measured. This value is almost identical to that measured for 3D randomly oriented IrMn.

Multiple Valley Modulations in Noncollinear Antiferromagnets.

Two-dimensional valleys and magnetism are rising areas with intriguing properties and practical uses in advanced information technology. By coupling valleys to collinear magnetism, valley degeneracy is lifted in a large number of magnetic valley materials to exploit the valley degree of freedom. Beyond collinear magnetism, new coupling modes between valley and magnetism are few but highly desirable. By tight-binding calculations of a breathing Kagome lattice, we demonstrate a tunable valley structure and valley-contrasting physical properties in noncollinear antiferromagnets. Distinct from collinear magnetism, noncollinear antiferromagnetic order enables valley splittings even without spin-orbit coupling. Both the canting and azimuthal angles of magnetic moments can be used as experimentally accessible knobs to tune valley splittings. Our first-principles calculations of the Fe3C6O6-silicene-Fe3C6O6 heterostructure also exhibit tunable valley splittings in noncollinear antiferromagnetism, agreeing with our tight-binding results. Our work paves avenues for designing novel magnetic valley materials and energy-efficient valleytronic devices based on noncollinear magnetism.

Single-Step Synthesis of An Ideal Chain Antiferromagnet [H2(4,4'-bipyridyl)](H3O)2Fe2F10 with Spin S = 5/2.

One-dimensional (1D) magnets are of great interest owing to their intriguing quantum phenomena and potential application in quantum computing. We successfully synthesized an ideal antiferromagnetic spin S = 5/2 chain compound [H2(4,4'-bpy)](H3O)2Fe2F10 (4,4'-bpy = 4,4'-bipyridyl) 1, using a single-step low-temperature hydrothermal method under conditions that favors the protonation of the bulky bidentate ligand 4,4'-bpy. Compound 1 consists of well-separated (Fe3+-F-)¥ chains with a large Fe-F-Fe angle of 174.8°. Both magnetic susceptibility and specific heat measurements show that 1 does not undergo a magnetic long-range ordering down to 0.5 K, despite the strong Fe-F-Fe intrachain spin exchange J with J/kB = -16.2(1) K. This indicates a negligibly weak interchain spin exchange J'. The J'/J value estimated for 1 is extremely small (< 2.8×10-6), smaller than those reported for all other S = 5/2 chain magnets. Our hydrothermal synthesis incorporates both [H2(4,4'-bpy)]2+ and (H3O)+ cations into the crystal lattice with numerous hydrogen bonds, hence effectively separating the (Fe3+-F-)¥ spin chains. This single-step hydrothermal synthesis under conditions favoring the protonation of bulky bidentate ligands offers an effective synthetic strategy to prepare well-separated 1D spin chain systems of magnetic ions with various spin values.

Ultrahigh Néel Temperature Antiferromagnetism and Ultrafast Laser-Controlled Demagnetization in a Dirac Nodal Line MoB3 Monolayer.

Two-dimensional (2D) antiferromagnetic (AFM) materials boasting a high Néel temperature (TN), high carrier mobility, and fast spin response under an external field are in great demand for efficient spintronics. Herein, we theoretically present the MoB3 monolayer as an ideal 2D platform for AFM spintronics. The AFM MoB3 monolayer features a symmetry-protected, 4-fold degenerate Dirac nodal line (DNL) at the Fermi level. It demonstrates a high magnetic anisotropy energy of 865 µeV/Mo and an ultrahigh TN of 1050 K, one of the highest recorded for 2D AFMs. Importantly, we reveal the ultrafast demagnetization of AFM MoB3 under laser irradiation, which induces a rapid transition from a DNL semimetallic state to a metallic state on the time scale of hundreds of femtoseconds. This work presents an effective method for designing advanced spintronics using 2D high-temperature DNL semimetals and opens up a new idea for ultrafast modulation of magnetization in topological semimetals.

Photocurrent Spectroscopy of Dark Magnetic Excitons in 2D Multiferroic NiI2.

Two-dimensional (2D) antiferromagnetic (AFM) semiconductors are promising components of opto-spintronic devices due to terahertz operation frequencies and minimal interactions with stray fields. However, the lack of net magnetization significantly limits the number of experimental techniques available to study the relationship between magnetic order and semiconducting properties. Here, they demonstrate conditions under which photocurrent spectroscopy can be employed to study many-body magnetic excitons in the 2D AFM semiconductor NiI2. The use of photocurrent spectroscopy enables the detection of optically dark magnetic excitons down to bilayer thickness, revealing a high degree of linear polarization that is coupled to the underlying helical AFM order of NiI2. In addition to probing the coupling between magnetic order and dark excitons, this work provides strong evidence for the multiferroicity of NiI2 down to bilayer thickness, thus demonstrating the utility of photocurrent spectroscopy for revealing subtle opto-spintronic phenomena in the atomically thin limit.

Chemical pressure induced spin reorientation in the magnetic structure ofCa3Mn2-xSnxO7(x=0,0.03,0.05).

The effect of partially substituting Tin (Sn) at the Manganese (Mn) site ofCa3Mn2O7, viz.Ca3Mn2-xSnxO7withx=0.03,0.05, on its structural and magnetic properties have been investigated using synchrotron diffraction, neutron diffraction, and bulk magnetization measurements. It is observed that with a substitution ofx=0.03, the minor (≈8%) tetragonal (I4/mmm) structural phase that is present in the predominantly orthorhombic (Cmc21) undopedCa3Mn2O7, completely disappears. The compounds order antiferromagnetically, the ordering temperature decreases with increasing Sn-content, indicating a weakening of the antiferromagnetic exchange interactions. Interestingly, in the ordered state, the spin magnetic moments which were aligned along thea-axis of the unit cell in the undoped compound, are observed to have reoriented with their major components lying in theb - cplane in the Sn-doped compounds. The above influence of Sn-doping is seen to be stemming from a significant modification of the octahedral rotation and tilt mode geometry in the unit cell, that is known to be responsible for driving ferroelectricity in these compounds.

Coexistence of Superconductivity and Antiferromagnetism in Topological Magnet MnBi2Te4 Films.

The interface of two materials can harbor unexpected emergent phenomena. One example is interface-induced superconductivity. In this work, we employ molecular beam epitaxy to grow a series of heterostructures formed by stacking together two nonsuperconducting antiferromagnetic materials, an intrinsic antiferromagnetic topological insulator MnBi2Te4 and an antiferromagnetic iron chalcogenide FeTe. Our electrical transport measurements reveal interface-induced superconductivity in these heterostructures. By performing scanning tunneling microscopy and spectroscopy measurements, we observe a proximity-induced superconducting gap on the top surface of the MnBi2Te4 layer, confirming the coexistence of superconductivity and antiferromagnetism in the MnBi2Te4 layer. Our findings will advance the fundamental inquiries into the topological superconducting phase in hybrid devices and provide a promising platform for the exploration of chiral Majorana physics in MnBi2Te4-based heterostructures.

Toward Fully Multiferroic van der Waals SpinFETs: Basic Design and Quantum Calculations.

Manipulating spin transport enhances the functionality of electronic devices, allowing them to surpass physical constraints related to speed and power. For this reason, the use of van der Waals multiferroics at the interface of heterostructures offers promising prospects for developing high-performance devices, enabling the electrical control of spin information. Our work focuses primarily on a mechanism for multiferroicity in two-dimensional van der Waals materials that stems from an interplay between antiferromagnetism and the breaking of inversion symmetry in certain bilayers. We provide evidence for spin-electrical couplings that include manipulating van der Waals multiferroic edges via external voltages and the subsequent control of spin transport including for fully multiferroic spin field-effect transistors.

Even-Odd Layer-Dependent Exchange Bias Effect in MnBi2Te4 Chern Insulator Devices.

Magnetic topological materials with coexisting magnetism and nontrivial band structures exhibit many novel quantum phenomena, including the quantum anomalous Hall effect, the axion insulator state, and the Weyl semimetal phase. As a stoichiometric layered antiferromagnetic topological insulator, thin films of MnBi2Te4 show fascinating even-odd layer-dependent physics. In this work, we fabricate a series of thin-flake MnBi2Te4 devices using stencil masks and observe the Chern insulator state at high magnetic fields. Upon magnetic field training, a large exchange bias effect is observed in odd but not in even septuple layer (SL) devices. Through theoretical calculations, we attribute the even-odd layer-dependent exchange bias effect to the contrasting surface and bulk magnetic properties of MnBi2Te4 devices. Our findings reveal the microscopic magnetic configuration of MnBi2Te4 thin flakes and highlight the challenges in replicating the zero magnetic field quantum anomalous Hall effect in odd SL MnBi2Te4 devices.

Interplay of lattice-spin-orbital coupling and Jahn-Teller effect in noncollinear spinel TixMn1-x(FeyCo1-y)2O4: a neutron diffraction study.

Local magnetostructural changes and dynamical spin fluctuations in doubly diluted spinel TixMn1‒x(FeyCo1‒y)2O4has been reported by means of neutron diffraction and magnetization studies. Two distinct sets of compositions (i)x(Ti) = 0.20 andy(Fe) = 0.18; (ii)x(Ti) = 0.40 andy(Fe) = 0.435 have been considered for this study. The first compound of equivalent stoichiometry Ti0.20Mn0.80Fe0.36Co1.64O4exhibits enhanced tetragonal distortion across the ferrimagnetic transition temperatureTC= 258 K in comparison to the end compound MnCo2O4(TC∼ 180 K) with a characteristic ratioct/√2atof 0.99795(8) demonstrating robust lattice-spin-orbital coupling. However, in the second case Ti0.40Mn0.60Fe0.87Co1.13O4with higherB-site compositions, the presence of Jahn-Teller ions with distinct behavior appears to counterbalance the strong tetragonal distortion thereby ceasing the lattice-spin-orbital coupling. Both the investigated systems show the coexistence of noncollinear antiferromagnetic and ferrimagnetic components in cubic and tetragonal settings. On the other hand, the dynamical ac-susceptibility,χac(T) reveals a cluster spin-glass state with Gabay-Toulouse (GT) like mixed phases behaviour belowTC. Such dispersive behaviour appears to be sensitive to the level of octahedral substitution. Further, the field dependence ofχac(T) follows the weak anisotropic GT-line behaviour with crossover exponent Φ lies in the range 1.38-1.52 on theH-Tplane which is in contrast to theB-site Ti substituted MnCo2O4spinel that appears to follow irreversible non-mean-field AT-line behaviour (Φ âˆ¼ 3 +δ). Finally, the Arrott plots analysis indicates the presence of a pseudo first-order like transition (T< 20 K) which is in consonance with and zero crossover of the magnetic entropy change within the frozen spin-glass regime.

The Impact of Local Strain Fields in Noncollinear Antiferromagnetic Films.

Antiferromagnets hosting structural or magnetic order that breaks time reversal symmetry are of increasing interest for "beyond von Neumann" computing applications because the topology of their band structure allows for intrinsic physical properties, exploitable in integrated memory and logic function. One such group are the noncollinear antiferromagnets. Essential for domain manipulation is the existence of small net moments found routinely when the material is synthesized in thin film form and attributed to symmetry breaking caused by spin canting, either from the Dzyaloshinskii-Moriya interaction or from strain. Although the spin arrangement of these materials makes them highly sensitive to strain, there is little understanding about the influence of local strain fields caused by lattice defects on global properties, such as magnetization and anomalous Hall effect. This premise is investigated by examining noncollinear antiferromagnetic films that are either highly lattice mismatched or closely matched to their substrate. In either case, edge dislocation networks are generated and for the former case, these extend throughout the entire film thickness, creating large local strain fields. These strain fields allow for finite intrinsic magnetization in seemingly structurally relaxed films and influence the antiferromagnetic domain state and the intrinsic anomalous Hall effect.

Charge-ordering breakdown dynamics and ferromagnetic resonance studies ofB-site Cu diluted Pr1‒xSrxMnO3.

Here, we report the influence of Jahn-Teller active Cu substitution on the charge-ordering (CO) characteristics of one of the well-known manganite Pr0.45Sr0.55MnO3(S55) with a distorted tetragonal structure. Magnetization studies unveil a complex magnetic phase diagram for S55, showing distinct temperature ranges corresponding to various magnetic phases: a ferromagnetic phase dominated by the Double Exchange interaction withTC∼ 220.5 K, an antiferromagnetic phase belowTN∼ 207.6 K induced by CO with a transition temperature ofTCO∼ 210 K consistent with the specific heatCP(T) data, and a mixed phase in the rangeTNTN(T

Quasi-2D spin-Peierls transition through interstitial anionic electrons in K(NH3)2.

Electron-phonon interactions and electron-electron correlations represent two crucial facets of condensed matter physics. For instance, in a half-filled spin-1/2 anti-ferromagnetic chain, the lattice dimerization induced by electron-nucleus interaction can be intensified by onsite Coulomb repulsion, resulting in a spin-Peierls state. Through first-principles calculations and crystal structure prediction methods, we have identified that under mild pressures, potassium and ammonia can form stable compounds: R3¯m K(NH3)2, Pm3¯m K(NH3)2, and Cm K2(NH3)3. Our predictions suggest that the R3¯m K(NH3)2 exhibits electride characteristics, marked by the formation of interstitial anionic electrons (IAEs) in the interlayer space. These IAEs are arranged in quasi-two-dimensional triangular arrays. With increasing pressure, the electronic van-Hove singularity shifts toward the Fermi level, resulting in an augmented density of states and the onset of both Peierls and magnetic instabilities. Analyzing these instabilities, we determine that the ground state of the R3¯m K(NH3)2 is the dimerized P21/m phase with zigzag-type anti-ferromagnetic IAEs. This state can be described by the triangular-lattice antiferromagnetic Heisenberg model with modulated magnetic interactions. Furthermore, we unveil the coexistence and positive interplay between magnetic and Peierls instability, constituting a scenario of spin-Peierls instability unprecedented in realistic 2D materials, particularly involving IAEs. This work provides valuable insights into the coupling of IAEs with the adjacent lattice and their spin correlations in quantum materials.

How to produce spin-splitting in antiferromagnetic materials.

Antiferromagnetic (AFM) materials have potential advantages for spintronics due to their robustness, ultrafast dynamics, and magnetotransport effects. However, the missing spontaneous polarization and magnetization hinders the efficient utilization of electronic spin in these AFM materials. Here, we propose a simple way to produce spin-splitting in AFM materials by making the magnetic atoms with opposite spin polarization locating in the different environment (surrounding atomic arrangement), which does not necessarily require the presence of spin-orbital coupling. We confirm our proposal by four different types of two-dimensional AFM materials within the first-principles calculations. Our works provide an intuitional design principle to find or produce spin-splitting in AFM materials.

Unveiling the Anomalous Hall Response of the Magnetic Structure Changes in the Epitaxial MnBi2Te4 Films.

Recently discovered as an intrinsic antiferromagnetic topological insulator, MnBi2Te4 has attracted tremendous research interest, as it provides an ideal platform to explore the interplay between topological and magnetic orders. MnBi2Te4 displays distinct exotic topological phases that are inextricably linked to the different magnetic structures of the material. In this study, we conducted electrical transport measurements and systematically investigated the anomalous Hall response of epitaxial MnBi2Te4 films when subjected to an external magnetic field sweep, revealing the different magnetic structures stemming from the interplay of applied fields and the material's intrinsic antiferromagnetic (AFM) ordering. Our results demonstrate that the nonsquare anomalous Hall loop is a consequence of the distinct reversal processes within individual septuple layers. These findings shed light on the intricate magnetic structures in MnBi2Te4 and related materials, offering insights into understanding their transport properties and facilitating the implementation of AFM topological electronics.

A Delicate Balance Between Spin-Wave Mediated Weak Localization and Electron-Phonon Scattering in the Design of Zero Temperature Coefficient of Resistivity.

Zero thermal coefficients of resistivity (ZTCR) materials exhibit minimal changes in resistance with temperature variations, making them essential in modern advanced technologies. The current ZTCR materials, which are based on the resistivity saturation effect of heavy metals, tend to function at elevated temperatures because the mean free path approaches the lower limit of the semiclassical Boltzmann theory when the temperature is sufficiently high. ZTCR materials working at low-temperatures are difficult to achieve due to electron-phonon scattering, which results in increased resistivity according to Bloch's theory. In this work, the ZTCR behavior at low-temperatures is realized in pre-microstrained Mn3NiN. The delicate balance between the resistivity contribution from electron-phonon scattering and spin-wave mediated weak localization is well revealed. A remarkable temperature coefficient of resistivity (TCR) value as low as 1.9 ppm K-1 (50 K ≤ T ≤ 200 K) is obtained, which is significantly superior to the threshold value of ZTCR behavior and the application standard of commercial ZTCR materials. The demonstration provides a unique paradigm in the design of ZTCR materials through the contraction effects of two opposite conductance mechanisms with positive and negative thermal coefficients of resistivity.

Recent progress in MnBi2nTe3n+1 intrinsic magnetic topological insulators: crystal growth, magnetism and chemical disorder.

The search for magnetic topological materials has been at the forefront of condensed matter research for their potential to host exotic states such as axion insulators, magnetic Weyl semimetals, Chern insulators, etc. To date, the MnBi2nTe3n+1 family is the only group of materials showcasing van der Waals-layered structures, intrinsic magnetism and non-trivial band topology without trivial bands at the Fermi level. The interplay between magnetism and band topology in this family has led to the proposal of various topological phenomena, including the quantum anomalous Hall effect, quantum spin Hall effect and quantum magnetoelectric effect. Among these, the quantum anomalous Hall effect has been experimentally observed at record-high temperatures, highlighting the unprecedented potential of this family of materials in fundamental science and technological innovation. In this paper, we provide a comprehensive review of the research progress in this intrinsic magnetic topological insulator family, with a focus on single-crystal growth, characterization of chemical disorder, manipulation of magnetism through chemical substitution and external pressure, and important questions that remain to be conclusively answered.

Phase Coexistence of Mn Trimer Clusters and Antiferromagnetic Mn Islands on Ir(111).

Clusters supported by solid substrates are prime candidates for heterogeneous catalysis and can be prepared in various ways. While mass-selected soft-landing methods are often used for the generation of monodisperse particles, self-assembly typically leads to a range of different cluster sizes. Here we show by scanning tunneling microscopy measurements that in the initial stages of growth, Mn forms trimers on a close-packed hexagonal Ir surface, providing a route for self-organized monodisperse cluster formation on an isotropic metallic surface. For an increasing amount of Mn, first a phase with reconstructed monolayer islands is formed, until at full coverage a pseudomorphic Mn phase evolves, which is the most densely packed one of the three different observed Mn phases on Ir(111). The magnetic state of both the reconstructed islands and the pseudomorphic film is found to be the prototypical antiferromagnetic Néel state with a 120° spin rotation between all nearest neighbors in the hexagonal layer.

Topological aspects of multi-kantiferromagnetism in cubic rare-earth compounds.

We advertise rare-earth intermetallics with high-symmetry crystal structures and competing interactions as a possible materials platform hosting spin structures with non-trivial topological properties. Focusing on the series of cubicRCu compounds, whereR= Ho, Er, Tm, the bulk properties of these systems display exceptionally rich magnetic phase diagrams hosting an abundance of different phase pockets characteristic of antiferromagnetic order in the presence of delicately balanced interactions. The electrical transport properties exhibit large anomalous contributions suggestive of topologically non-trivial winding in the electronic and magnetic structures. Neutron diffraction identifies spontaneous long-range magnetic order in terms of commensurate and incommensurate variations of(ππ0)antiferromagnetism with the possibility for various multi-kconfigurations. Motivated by general trends in these materials, we discuss the possible existence of topologically non-trivial winding in real and reciprocal space in the class ofRCu compounds including antiferromagnetic skyrmion lattices. Putatively bringing together different limits of non-trivial topological winding in the same material, the combination of properties inRCu systems promises access to advanced functionalities.

2D Co-Directed Metal-Organic Networks Featuring Strong Antiferromagnetism and Perpendicular Anisotropy.

Antiferromagnetic spintronics is a rapidly emerging field with the potential to revolutionize the way information is stored and processed. One of the key challenges in this field is the development of novel 2D antiferromagnetic materials. In this paper, the first on-surface synthesis of a Co-directed metal-organic network is reported in which the Co atoms are strongly antiferromagnetically coupled, while featuring a perpendicular magnetic anisotropy. This material is a promising candidate for future antiferromagnetic spintronic devices, as it combines the advantages of 2D and metal-organic chemistry with strong antiferromagnetic order and perpendicular magnetic anisotropy.