Magnetic Atoms Research Articles

Atomic-scale magnetic doping of monolayer stanene by revealing Kondo effect from self-assembled Fe spin entities

Atomic-scale spin entity in a two-dimensional topological insulator lays the foundation to manufacture magnetic topological materials with single atomic thickness. Here, we have successfully fabricated Fe monomer, dimer and trimer doped in the monolayer stanene/Cu(111) through a low-temperature growth and systematically investigated Kondo effect by combining scanning tunneling microscopy/spectroscopy (STM/STS) with density functional theory (DFT) and numerical renormalization group (NRG) method. Given high spatial and energy resolution, tunneling conductance (dI/dU) spectra have resolved zero-bias Kondo resonance and resultant magnetic-field-dependent Zeeman splitting, yielding an effective spin Seff = 3/2 with an easy-plane magnetic anisotropy on the self-assembled Fe atomic dopants. Reduced Kondo temperature along with attenuated Kondo intensity from Fe monomer to trimer have been further identified as a manifestation of Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction between Sn-separated Fe atoms. Such magnetic Fe atom assembly in turn constitutes important cornerstones for tailoring topological band structures and developing magnetic phase transition in the single-atom-layer stanene.

Influence of the Cooling Rate on the Heterogeneity of the Structure in the Rapid Quenched Fe – Based Alloys with the Si Addition

The paper presents the results of research from the analysis of primary magnetization curves for Fe based amorphous alloys. Structural defects in the form of pseudodislocation dipoles occur in amorphous alloys. Using the theory developed by H. Kronmuller called the approach to ferromagnetic saturation, it is possible to indirectly observe internal stresses occurring in the volume of amorphous alloys. The magnetic structure is sensitive to all kinds of inhomogeneities that become visible in the process of high-field magnetization. It has been shown that the cooling rate of the liquid alloy has a great influence on the migration of atoms during the solidification process. Longer time of alloy formation causes more atoms to occupy ordered positions, which results in a change in the distance between the magnetic atoms and a higher degree of structure relaxation. This is indicated by a significant difference in the value of the spin wave stiffness parameter Dspf. The structural differences of the alloys were also investigated using a magnetic balance. It has been shown that the cooling rate influences insignificant differences in the course of thermomagnetic curves and the Curie temperature.

Landau Levels versus Hydrogen Atom

The Landau problem and harmonic oscillator in the plane share a Hilbert space that carries the structure of Dirac’s remarkable so(2,3) representation. We show that the orthosymplectic algebra osp(1|4) is the spectrum generating algebra for the Landau problem and, hence, for the 2D isotropic harmonic oscillator. The 2D harmonic oscillator is in duality with the 2D quantum Coulomb–Kepler systems, with the osp(1|4) symmetry broken down to the conformal symmetry so(2,3). The even so(2,3) submodule (coined Rac) generated from the ground state of zero angular momentum is identified with the Hilbert space of a 2D hydrogen atom. An odd element of the superalgebra osp(1|4) creates a pseudo-vacuum with intrinsic angular momentum 1/2 from the vacuum. The odd so(2,3)-submodule (coined Di) built upon the pseudo-vacuum is the Hilbert space of a magnetized 2D hydrogen atom: a quantum system of a dyon and an electron. Thus, the Hilbert space of the Landau problem is a direct sum of two massless unitary so(2,3) representations, namely, the Di and Rac singletons introduced by Flato and Fronsdal.

Magnetic behaviour of a mixed-spin ising model on a two-dimensional square-octagon lattice in a dynamic magnetic field

The magnetic behaviours of a two-dimensional square-octagon lattice with mixed spin 5/2 and spin 1 magnetic atoms are investigated in a dynamic magnetic field using effective field theory with correlations. We studied the effects of exchange coupling, anisotropy, oscillating magnetic fields, and temperature on the dynamic magnetic and thermodynamic properties of the square-octagon lattice. The dynamic magnetisation, order parameters, susceptibility, internal energy, and phase diagram of the system were obtained. These results significantly contribute to our understanding of the dynamic magnetic properties of two-dimensional materials. The ability to manipulate and control magnetic behaviour in two dimensions holds promise for the creation of more efficient and versatile devices.

Topological stability of spin textures in Si/Co-doped helimagnet FeGe

Element substitutions with magnetic or non-magnetic atoms are known to significantly impact the magnetic structure and related transport properties of magnets. To clarify the change of magnetic structure of B20-type magnets with element doping, we conduct real-space observations of spin textures and their temperature (T)-magnetic field (H) phase diagrams of a helimagnet FeGe with partially substituting Fe and Ge with Co and Si, respectively. The helical period (λ) changes dramatically by the element doping: λ increases by 147% to 103 nm in 30% Co-doped FeGe, whereas it decreases by around 70% to 49 nm in 30% Si-doped FeGe, compared to the λ =70 nm in FeGe. Upon applying the magnetic field normally to (001), (110), and (111) thin plates of both FeSi0.3Ge0.7 and Fe0.7Co0.3Ge, the hexagonal skyrmion crystal (SkX) state emerges. The magnetic phase diagrams observed through the real-space imaging reveal that (1) the SkX can extend to a larger T-H window by reducing the sample thickness or by cooling the sample under specific magnetic fields from temperatures above the transition temperature (TC ); (2) the stability of the SkX phase differs between Si-doped and Co-doped FeGe: the SkX phase is most unstable in the (111) FeSi0.3Ge0.7, while it remains robust in the (111) Fe0.7Co0.3Ge. These differences indicate distinct anisotropic behavior in FeGe with magnetic (Co) and non-magnetic-element (Si) dopants.

Electrically controlled nonvolatile switching of single-atom magnetism in a Dy@C84 single-molecule transistor

Single-atom magnetism switching is a key technique towards the ultimate data storage density of computer hard disks and has been conceptually realized by leveraging the spin bistability of a magnetic atom under a scanning tunnelling microscope. However, it has rarely been applied to solid-state transistors, an advancement that would be highly desirable for enabling various applications. Here, we demonstrate realization of the electrically controlled Zeeman effect in Dy@C84 single-molecule transistors, thus revealing a transition in the magnetic moment from 3.8 μB\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${\\mu }_{{{{{{\\rm{B}}}}}}}$$\\end{document} to 5.1 μB\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${\\mu }_{{{{{{\\rm{B}}}}}}}$$\\end{document} for the ground-state GN at an electric field strength of 3−\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$-$$\\end{document}10 MV/cm. The consequent magnetoresistance significantly increases from 600% to 1100% at the resonant tunneling point. Density functional theory calculations further corroborate our realization of nonvolatile switching of single-atom magnetism, and the switching stability emanates from an energy barrier of 92 meV for atomic relaxation. These results highlight the potential of using endohedral metallofullerenes for high-temperature, high-stability, high-speed, and compact single-atom magnetic data storage.

Stabilization of Hubbard-Thouless pumps through nonlocal fermionic repulsion

Thouless pumping represents a powerful concept to probe quantized topological invariants in quantum systems. We explore this mechanism in a generalized Rice-Mele Fermi-Hubbard model characterized by the presence of competing onsite and intersite interactions. Contrary to recent experimental and theoretical results, showing a breakdown of quantized pumping induced by the onsite repulsion, we prove that sufficiently large intersite interactions allow for an interaction-induced recovery of Thouless pumps. Our analysis further reveals that the occurrence of stable topological transport at large interactions is connected to the presence of a spontaneous bond-order-wave in the ground-state phase diagram of the model. Finally, we discuss a concrete experimental setup based on ultracold magnetic atoms in an optical lattice to realize the newly introduced Thouless pump. Our results provide a new mechanism to stabilize Thouless pumps in interacting quantum systems.

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.

Theory for magnetic impurity modes in two-dimensional van der Waals ferromagnetic films

A spin-wave analysis is developed to calculate the energies of the localized excitations occurring in two-dimensional ferromagnetic van der Waals monolayers when a substitutional magnetic impurity is introduced. The magnetic ions lie on a bipartite honeycomb lattice (similar to that for graphene) and the theory includes the effects of both Ising anisotropy and single-ion anisotropy to stabilize the magnetic ordering perpendicular to the atomic plane at low temperatures. A Dyson-equation formalism, together with the spin-dependent Green’s functions derived for van der Waals monolayers, is employed to evaluate the existence conditions and energies for the impurity modes, which lie above the band of spin-wave states of the pure host material. For realistic parameter values it is found that typically two impurity modes may exist, depending on the spin quantum number for the magnetic impurity atom. Numerical applications are made to CrI3 and Cr2Ge2Te6 as the host materials.

An Atomic-Scale Vector Network Analyzer.

Electronic devices have been ever-shrinking toward atomic dimensions and have reached operation frequencies in the GHz range, thereby outperforming most conventional test equipment, such as vector network analyzers (VNA). Here the capabilities of a VNA on the atomic scale in a scanning tunneling microscope are implemented. Nonlinearities present in the voltage-current characteristic of atoms and nanostructures for phase-resolved microwave spectroscopy with unprecedented spatial resolution at GHz frequencies are exploited. The amplitude and phase response up to 9.3GHz is determined, which permits accurate de-embedding of the transmission line and application of distortion-corrected waveforms in the tunnel junction itself. This enables quantitative characterization of the complex-valued admittance of individual magnetic iron atoms which show a lowpass response with a magnetic-field-tunable cutoff frequency.

Observation of Topological Hall Effect in a Chemically Complex Alloy.

The topological Hall effect (THE) is the transport response of chiral spin textures and thus can serve as a powerful probe for detecting and understanding these unconventional magnetic orders. So far, the THE is only observed in either noncentrosymmetric systems where spin chirality is stabilized by Dzyaloshinskii-Moriya interactions, or triangular-lattice magnets with Ruderman-Kittel-Kasuya-Yosida-type interactions. Here, a pronounced THE is observed in a Fe-Co-Ni-Mn chemically complex alloy with a simple face-centered cubic (fcc) structure across a wide range of temperatures and magnetic fields. The alloy is shown to have a strong magnetic frustration owing to the random occupation of magnetic atoms on the close-packed fcc lattice and the direct Heisenberg exchange interaction among atoms, as evidenced by the appearance of a reentrant spin glass state in the low-temperature regime and the first principles calculations. Consequently, THE is attributed to the nonvanishing spin chirality created by strong spin frustration under the external magnetic field, which is distinct from the mechanism responsible for the skyrmion systems, as well as geometrically frustrated magnets.

Transport Properties with Multiple Functions of Fe@C60-GNR Single Molecule.

Encouraged by the successful fabrication of C60-GNR (GNR=graphene nanoribbon) single-molecule transistors in experiments, four Fe-containing derived double-layered devices of Fe@C60-GNR are designed by employing different electrode linkages and their transport properties are investigated by using density functional theory (DFT) and nonequilibrium Green's function (NEGF) methods. Regardless of electrode connection, all these devices give rise to a smaller negative differential resistance (NDR) peak at V=0.2 and a higher peak at 1.2 V, suggesting their stable maneuverability as molecular devices and good candidates for developing on(off)-off(on)-on(off) current switches. The macroscopic NDR performance depends on the delocalization character and the crossing mechanism of the frontier orbitals. The peak-to-valley current ratios (Rmax) range from 454 to 2737, determined by the electrode linkage. Such a large Rmax-value is necessary for developing dynamic random-access memory (DRAM) cells. Encapsulating the Fe atom inside C60 not only improves the conductivity but also introduces the spin-polarized transport property. The spin-filtering efficiency (SFE) of almost all devices oscillates up and down in response to the bias voltage, indicating the possibility of designing on(off)-off(on)-on(off) spin switches and up-down spin switches. All these fascinating properties provide an important clue for designing similar molecular devices with multiple functions by trapping magnetic transition metal atoms inside fullerenes.

Ultrafast spin dynamics in magnetic trimer and tetramer clusters: a step towards prototypic spin-SHIFT registers

Ultrafast magnetic dynamics is a necessary ingredient for magnetic recording and ultrafast information processing. The shift functionality, although not mandatory for Boolean logic, is always implemented in CMOS CPUs and therefore must be also present in magnetic logic. In this respect, using ab initio calculations we show ultrafast spin dynamics in molecular clusters such as Co3 +CO and Ni4. In this work, we establish that clusters with magnetic atoms can provide a theoretical toolbox for efficient spin charge dynamics whose operation time can range up to a few picoseconds. The prime underlying mechanism for all spin manipulation scenarios in the above mentioned clusters are laser-induced Λ processes where the laser parameters are fully optimized using a genetic algorithm. In general, a structural asymmetry enforces substantial spin localization on the active centers of both magnetic clusters. Keeping in mind the shift functionality, we theoretically suggest a series of spin-transfer scenarios between the Co and Ni atoms in each of these two clusters independently to construct a 3-bit and a 4-bit cyclic spin-SHIFT register, respectively. The maximum operational time for both logic devices is 2 ps, which is much faster than the response time of conventional spintronic devices. Additionally, for a better understanding of the transfer cycles, their feasibility and reversibility are also investigated through the analysis of the optical spectra of the related states. Our results provide important theoretical guidance for ultrafast spin manipulation in molecular structures as well as their potential spin functionality, and thus step closer to the realization of future spin-based logic devices and quantum computation. This effectively motivates the investigation and precise establishment of the shift functionality in magnetic trimers and tetramers.

Fe3O4/PMMA with Well-Arranged Structures Synthesized through Magnetic Field-Assisted Atom Transfer Radical Polymerization.

Particle- or fiber-reinforced polymer composites with controlled orientations are attracting interest and applications producing innovative materials, biological constructs, and energy devices. To gain the controlled orientations, filed-assisted synthesis is widely selected for its easy operation and control. In this paper, we designed magnetic field-assisted equipment and synthesized a magnetic polymer composite Fe3O4/PMMA with a well-arranged layers structure by combining the magnetic field with atom transfer radical polymerization (ATRP). During the polymerization of polymer composites, the magnetic nanoparticles were surrounded by monomers. With the growth of polymer chains, the magnetic particles pushed polymer chains to move according to a specific direction and form a well-arranged structure under the magnetic fields. The existence of a well-arranged layered structure of the composites gives potential guidance for controlling the micro-structure by adding an extra field during the polymerization process. The experimental results provided a possible design to influence the macroscale properties through control of the micro-structure of polymer composites.

Experimental observation of purely resistive effect in epsilon-near-zero transition metal perovskite

The epsilon-near-zero (ENZ) properties of nanomaterials provide a promising paradigm for the development of next-generation nanoscale electronic devices, especially in 6 G communication systems. However, realizing ENZ in the radio frequency (RF) domain remains a challenge due to the scarcity of materials. Here, a strategy is proposed to exploit the intrinsic excitation of polarons and delocalized electrons to modify the carrier dynamics in transition metal perovskite for tailored dielectric response in the RF domain. Polarons and delocalized electrons are introduced into the material through lattice distortion and exchange mechanisms between magnetic atoms, and are precisely governed. The tunable kHz-band ENZ is realized in La0.90Ba0.10CoO3 and described using the Debye-Drude model. Importantly, the purely resistive effect is experimentally observed under ENZ condition, manifesting as near-zero reactance and phase angle, which is attributed to the inductor-capacitor resonance through equivalent circuit analysis. These findings provide a new avenue for implementing ENZ at RF domain and identify transition metal perovskites as ENZ candidates.

Strain-tunable ferromagnetism and skyrmions in two-dimensional Janus Cr2XYTe6 (X, Y = Si, Ge, Sn, and X≠Y) monolayers

By using first-principles calculations and micromagnetic simulations, we investigate the electronic structure, magnetic properties, and skyrmions in two-dimensional Janus Cr2XYTe6 (X,Y = Si, Ge, Sn, X ≠ Y) monolayers. Our findings reveal that the Cr2XYTe6 monolayers are ferromagnetic semiconductors with a high Curie temperature (Tc). The bandgap and Tc can be further increased by applying tensile strain. In addition, there is a transition from the ferromagnetic to the antiferromagnetic state at a compressive strain. Both Cr2SiSnTe6 and Cr2SiGeTe6 exhibit a large magnetic anisotropy energy, which are mainly associated with the significant spin–orbit coupling of the nonmagnetic Te atoms rather than that of the magnetic Cr atoms. Interestingly, the Cr2SiSnTe6 monolayer exhibits a significant Dzyaloshinskii–Moriya interaction of 1.12 meV, which facilitates the formation of chiral domain walls and skyrmions. Furthermore, under tensile strain, chiral DWs can be transformed into skyrmions if applying an external magnetic field. These findings suggest that Janus Cr2XYTe6 monolayers hold promise for spintronic nanodevice applications.

DFT and Monte Carlo investigations of electronic structure, magnetic, magnetocaloric, and thermoelectric properties of the perovskite SrXO3 (X = Mn and Fe) compound

The structural, electronic, magnetic, magnetocaloric, and thermoelectric properties of the SrXO3 (X = Mn and Fe) perovskite compounds were investigated using first-principles calculations. It was observed that the SrXO3 compounds are G-anti-ferromagnetic perovskites with partial magnetic moment with a value of 2.7 [Formula: see text] and 2.4 [Formula: see text] for Mn-3d and Fe-3d orbitals for SrMnO3 and SrFeO3, respectively. Moreover, by using Monte Carlo simulation (MCs) combined with the Metropolis algorithm, the calculated coupling interactions between the magnetic atoms Mn–Mn and Fe–Fe are [Formula: see text][Formula: see text]meV and [Formula: see text][Formula: see text]meV for SrMnO3, [Formula: see text][Formula: see text]meV and [Formula: see text][Formula: see text]meV for SrFeO3, respectively. Furthermore, a significant magnetocaloric effect (MCE) was observed around the Néel temperature of [Formula: see text][Formula: see text]K (for SrMnO3) and [Formula: see text][Formula: see text]K (for SrFeO3), and the maximal simulated magnetic entropy and relative cooling power values of all the studied compounds are found to be 100[Formula: see text]J/kg (for SrMnO3) and 110[Formula: see text]J/kg (for SrFeO3), respectively, with an applied magnetic field of [Formula: see text] T. These results are in complete agreement with the experimental results and more specifics than other theoretical calculations. Hence, SrXO3 compounds are considered promising candidates for magnetic refrigeration at low temperature.

Enhancement of single-atom catalytic activity by the synergistic effect of interlayer charge transfer and magnetic coupling in an electride-based heterostructure.

2D material-based single-atom catalysts have rapidly emerged and flourished in recent years due to their exceptional atomic utilization efficiency, adjustable catalytic activity, and remarkably high selectivity. The interface matching mechanism of 2D materials, influenced by van der Waals (vdW) interactions, presents a novel opportunity for constructing a heterostructure, further augmenting catalytic efficiency. In this work, the mechanism of performance regulation of magnetic transition-metal decorated MoS2 single-atom catalysis by importing a Gd2C electride substrate is investigated using first-principles calculations. The localization of d orbitals in transition-metals is weakened by adding a Gd2C substrate, thereby modulating the catalytic performance. Our findings demonstrate that the formation of an electron layer at the interface of the heterostructure by electride Gd2C induces a modification in the chemical environment of the MoS2 surface. The electron layer enhances the electron transfer during catalysis. Additionally, for the catalyst containing magnetic atoms, Gd2C can also achieve catalytic performance adjustment due to the magnetic coupling, similar to the effect of external magnetic fields. This study offers a novel concept and a pathway for enhancing the performance of single-atom catalysts through the construction of a heterostructure, capitalizing on the distinctive electron layer of an electride and its inherent high magnetic moments.

Inducing abundant magnetic phases and enhancing magnetic stability by edge modifications and physical regulations for NiI2 nanoribbons.

Recently, a magnetic semiconducting NiI2 monolayer was successfully fabricated. To obtain richer magneto-electronic properties and find new physics for NiI2, we studied the zigzag-type NiI2 nanoribbon (ZNiI2NR) with edges modified by different concentrations of H and/or O atoms. Results show that these ribbons hold a higher energy stability, thermal stability, and magnetic stability, and the Curie temperature can be increased to 143 from 15 K for the bare-edged ribbons. They feature a half-semiconductor, bipolar magnetic semiconductor, or half-metal, depending on the edge-terminated atomic species and concentrations, and are closely related to the ribbon edge states, impurity bands or hybridized bands. By applying strain or an electric field, ribbons can achieve a reversible multi-magnetic phase transition among a bipolar magnetic semiconductor, half-semiconductor, half-metal, and magnetic metal. This is because strain changes the Ni-I bond length, resulting in a variation of bond configurations (weight of ionic and covalent bonds) and the number of unpaired electrons. The compressive strain can increase the Curie temperature because it makes the edged Ni-I-Ni bond angle closer to 90°, leading to the FM d-p-d superexchange interaction being increased. The electric field varies the magnetic phase because it alters the electrostatic potential of the ribbon edges, and the Curie temperature is enhanced under the electric field because the ribbon is changed to a metallic state (half-metal or magnetic metal), in which the magnetic Ni atoms satisfy the Stoner criterion and hold a large magnetic exchange coefficient and electron state density at the Fermi surface.

Investigation of the lattice thermal transport properties of Janus XClO (X = Cr, Ir) monolayers by first-principles calculations.

In the context of the global energy crisis, the development of high-performance heat transport devices within nano scales has become increasingly important. Theoretical discovery and evaluation of novel structures with high performance in thermal conductivity by affordable calculations could provide significant instructions for experimental studies focusing on thermoelectric device development. For 2-dimensional (2D) functional materials, their heat transport efficiency is correlated with their electronic properties and structural features. In this study, we computationally investigated the heat transport within Janus XClO (X = Cr, Ir); its structural and electronic properties were well solved by first-principles calculations. Furthermore, to evaluate thermodynamics stability and applicability, ab initio molecular dynamics (AIMD) simulations are conducted. Through a benchmarking study upon these XClO monolayers with different compositions, we noticed that their heat transport efficiency is associated with the percentage of doped magnetic atoms. The theoretical insights provided by this study are highly instructive for future experimental studies focusing on thermal device development.