Atomic Spin Research Articles

Ferromagnetism on an atom-thick & extended 2D metal-organic coordination network

Ferromagnetism is the collective alignment of atomic spins that retain a net magnetic moment below the Curie temperature, even in the absence of external magnetic fields. Reducing this fundamental property into strictly two-dimensions was proposed in metal-organic coordination networks, but thus far has eluded experimental realization. In this work, we demonstrate that extended, cooperative ferromagnetism is feasible in an atomically thin two-dimensional metal-organic coordination network, despite only ≈ 5% of the monolayer being composed of Fe atoms. The resulting ferromagnetic state exhibits an out-of-plane easy-axis square-like hysteresis loop with large coercive fields over 2 Tesla, significant magnetic anisotropy, and persists up to TC ≈ 35 K. These properties are driven by exchange interactions mainly mediated by the molecular linkers. Our findings resolve a two decade search for ferromagnetism in two-dimensional metal-organic coordination networks.

Indication of critical scaling in time during the relaxation of an open quantum system

Near continuous phase transitions, universal power-law scaling, characterized by critical exponents, emerges. This behavior reflects the singular responses of physical systems to continuous control parameters like temperature or external fields. Universal scaling extends to non-equilibrium dynamics in isolated quantum systems after a quench, where time takes the role of the control parameter. Our research unveils critical scaling in time also during the relaxation dynamics of an open quantum system. Here we experimentally realize such a system by the spin of individual Cesium atoms dissipatively coupled through spin-exchange processes to a bath of ultracold Rubidium atoms. Through a finite-size scaling analysis of the entropy dynamics via numerical simulations, we identify a critical point in time in the thermodynamic limit. This critical point is accompanied by the divergence of a characteristic length, which is described by critical exponents that turn out to be unaffected by system specifics.

Critical characteristics of spin − 1/2 four-leg nanotube: Monte Carlo Simulation

In this study, we aim to investigate theoretically the critical characteristics of spin −1/2 four-leg nanotube for the nanotechnology applications. The Ising model simulated by Monte Carlo simulation is adopted with the first exchange coupling J , the second exchange coupling between the second nearest neighbor atomic spins J ′ and the transverse exchange coupling J z , and the external magnetic field h as parameters. Herein, we examine the local properties of spin −1/2 four-leg nanotube by analyzing the magnetization, susceptibility and hysteresis loop behavior as function of J ′ , J Z and h . The obtained results show that the isotropic ‐ 1 / 2 four-leg nanotube Ising model presents critical behavior at ferromagnetic to paramagnetic phase transition where the Curie temperature T C increases according to vertical and second nearest neighbor exchange coupling. Furthermore, under external magnetic field, the magnetization keeps the second order transition and the magnetic susceptibility declines with the increase of applied external magnetic field value. In addition to that, we have found single ferromagnetic hysteresis loops, for which the shape increases by increasing the second nearest neighbor exchange coupling when T = J . Finally, the critical temperature shows perfect mirror symmetry relative to the vertical and increases with the second nearest neighbor exchange coupling.

Conventional and Unconventional Dicke Models: Multistabilities and Nonequilibrium Dynamics.

The Dicke model describes the collective behavior of a subwavelength-size ensemble of two-level atoms (i.e., spin-1/2) interacting identically with a single quantized radiation field of a cavity. Across a critical coupling strength it exhibits a zero-temperature phase transition from the normal state to the superradiant phase where the field is populated and the collective spin acquires a nonzero x component, which can be imagined as ferromagnetic ordering of the atomic spins along x. Here we introduce a variant of this model where two subwavelength-size ensembles of spins interact with a single quantized radiation field with different strengths. Subsequently, we restrict ourselves to a special case where the coupling strengths are opposite (which is unitarily equivalent to equal-coupling strengths). Because of the conservation of the total spin in each ensemble individually, the system supports two distinct superradiant states with x-ferromagnetic and x-ferrimagnetic spin ordering, coexisting with each other in a large parameter regime. The stability and dynamics of the system in the thermodynamic limit are examined using a semiclassical approach, which predicts nonstationary behaviors due to the multistabilities. At the end, we also perform small-scale full quantum-mechanical calculations, with results consistent with the semiclassical ones.

Single-shot all-optical switching of magnetization in TbFe

Thermally induced magnetization switching (TIMS) relying solely on a single laser without any applied magnetic field is a key research direction of current spintronics. Most studies on TbFe so far have focused on helicity-dependent all-optical switching (HD-AOS). In this work, we observe the TIMS on TbFe alloys excited by atomic spin dynamics simulations combined with a two-temperature model. The results show that the magnetization switching of TbFe can be found under certain damping conditions. In addition, we further investigated the reasons why energy density leads to the opposite switching time behavior of Tb and Fe, and our research results also found that changes in damping can affect the concentration and energy density range of the switching, as well as the maximum pulse duration. The dynamic behavior indicates that TbFe switching in 2 ps or less. Our findings widen the basis for fast optical switching of magnetization and break new ground for engineered materials that can be used for nonvolatile ultrafast switching using ultrashort pulses of light.

Approaching a fully-polarized state of nuclear spins in a solid

Magnetic noise of atomic nuclear spins is a major source of decoherence in solid-state spin qubits. In theory, near-unity nuclear spin polarization can eliminate decoherence of the electron spin qubit, while turning the nuclei into a useful quantum information resource. However, achieving sufficiently high nuclear polarizations has remained an evasive goal. Here we implement a nuclear spin polarization protocol which combines strong optical pumping and fast electron tunneling. Nuclear polarizations well above 95% are generated in GaAs semiconductor quantum dots on a timescale of 1 minute. The technique is compatible with standard quantum dot device designs, where highly-polarized nuclear spins can simplify implementations of qubits and quantum memories, as well as offer a testbed for studies of many-body quantum dynamics and magnetism.

Spectral analysis of spin noise in an optically spin-polarized stochastic Bloch equation driven by noisy magnetic fields

We theoretically analyze an optically spin-polarized collection of atoms, which serves as a basis for atomic sensors. Assuming that the intrinsic atomic spin projection noise is negligible, we provide the closed-form autocorrelation function and the power spectral density (PSD) of the solution to a noisy version of an optically pumped Bloch equation, wherein each component of the external magnetic field is subjected to white noise. We conclude that noise in the bias B-field direction does not affect the autocorrelation function, up to first order in white noise covariance amplitudes. Moreover, the noise terms for the remaining two axes make different contributions to the magnetic noise-driven spin PSD; in particular, the contribution corresponding to noises perpendicular to the probing direction dominates at high frequencies. Some results concerning the second (and higher)-order terms are given. In particular, we anticipate a decrease in the effective Larmor frequency despite an increase in the magnetic field magnitude in the case of anisotropic transversal B-field noises. The analytic results are supported by Monte Carlo simulations employing the Euler–Maruyama method. The analytic methodology is applied to the case of a Bell–Bloom magnetometer, which reveals a non-linearity in the PSD of the magnetometer output and also a broadening effect due to magnetic field noise.

Real-time quantum control of spin-coupling damping and application in atomic spin gyroscopes

Real-time quantum control of spin-coupling damping and application in atomic spin gyroscopes

Separating the contributions of the magnetic subsystems in antiferromagnetic ferrihydrite nanoparticles by analyzing the magnetization in fields of up to 250 kOe

Contributions of different magnetic subsystems formed in the systems of synthetic ferrihydrite nanoparticles (characterized previously) with an average size of < d>≈2.7 nm coated with polysaccharide arabinogalactan in different degrees have been separated by measuring the dependences of their magnetization M on magnetic field H of up to 250kOe on vibrating sample and pulsed magnetometers. The use of a wide measuring magnetic field range has been dictated by the ambiguity in identifying a linear M(H) portion for such antiferromagnetic nanoparticle systems within the conventional field range of 60–90 kOe. The thorough analysis of the magnetization curves in the temperature range of 100–250 K has allowed the verification of the contributions of (i) uncompensated magnetic moments µun in the superparamagnetic subsystem, (ii) the subsystem of surface spins with the paramagnetic behavior, and (iii) the antiferromagnetic susceptibility of the antiferromagnetically ordered ferrihydrite particle core. As a result, a model of the magnetic state of ferrihydrite nanoparticles has been proposed and the numbers of spins corresponding to magnetic subsystems (i)–(iii) have been estimated. An average magnetic moment μunof ∼ 145μB (μB is the Bohr magneton) per particle corresponds approximately to 30 decompensated spins of iron atoms in a particle (about 3 % of all iron atoms), which, according to the Néel’s hypothesis μun∼<d>3/2, are localized both on the surface and in the bulk of an antiferromagnetically ordered particle. The fraction of free (paramagnetic) spins is minimal in the sample without arabinogalactan coating of the nanoparticle surface (7 %) and is attained 20 % of all iron atoms in the sample with the highest degree of spatial separation of particles. According to this estimation, paramagnetic spins are located mainly on the edges and protruding areas of particles. Most magnetic moments of iron atoms are ordered antiferromagnetically and the corresponding magnetic susceptibility of this subsystem behaves as in an antiferromagnet with the randomly distributed crystallographic axes, i.e., increases with temperature.

Investigation of Floquet engineered non-Abelian geometric phase for holonomic quantum computing

Holonomic quantum computing functions by transporting an adiabatically degenerate manifold of computational states around a closed loop in a control-parameter space; this cyclic evolution results in a non-Abelian geometric phase which may couple states within the manifold. Realizing the required degeneracy is challenging and typically requires auxiliary levels or intermediate-level couplings. One potential way to circumvent this is through Floquet engineering, where the periodic driving of a nondegenerate Hamiltonian leads to degenerate Floquet bands, and subsequently non-Abelian gauge structures may emerge. Here we present an experiment in ultracold Rb87 atoms where atomic spin states are dressed by modulated RF fields to induce periodic driving of a family of Hamiltonians linked through a fully tuneable parameter space. The adiabatic motion through this parameter space leads to the holonomic evolution of the degenerate spin states in SU(2), characterized by a non-Abelian connection. We study the holonomic transformations of spin eigenstates in the presence of a background magnetic field, characterizing the fidelity of these single-qubit gate operations. Results indicate that while the Floquet engineering technique removes the need for explicit degeneracies, it inherits many of the same limitations present in degenerate systems. Published by the American Physical Society 2024

Effect of the Interaction between Transition Metal Redox Center and Cyanide Ligand on Structural Evolution in Prussian White Cathodes.

Transition metal (TM) based Prussian whites, comprising a cyanide anion ((C≡N)-) and TM cations in an alternative manner, have been widely adopted as cathode materials for rechargeable batteries. Prussian whites are characterized by the TM electronic states that exclusively adopt low spin (LS) toward the C atom and high spin (HS) toward the N atom through the hybridized covalent bonding in the TM─C≡N─TM unit with the average oxidation states of the TM ions being 2+, considerably affecting the phase transition behavior upon the release and storage of carrier ions; however, there have been only a few studies on their associated features. Herein, Prussian whites with different HS TM ions were synthesized via coprecipitation and the phase transition behavior controlled by the π electron interaction between the cyanide anions and TM ions during battery operations was investigated. In situ X-ray characterizations reveal that the combined effect of π backdonation in the LS Fe-C unit and π donation in the HS TM-N unit effectively controls the bond length of the TM─C≡N─TM building unit, thus markedly influencing the lattice volume of a series of Prussian white cathodes during the charge/discharge process. This study presents a comprehensive understanding of the structure-property relationship of the Prussian white cathodes involving π electron interactions during battery operations.

Моделирование процессов формирования и исследование свойств нанопленок Co-Fe-Nb

The article presents the study of the formation and the analysis of the structure and properties of nanomaterials, which are cobalt-iron-niobium thin-film systems. A mathematical model is presented that allows to describe the combined behavior of atomic spins and coordinates. The generalized version of the model can use any type of the force interaction potential and take into account various contributions to the magnetic Hamiltonian depending on the specific problem being solved. When conducting computational experiments, the force potential of the modified embedded atom method (MEAM) was considered; to take into account magnetic interactions, a simplified magnetic Hamiltonian that includes the exchange interaction and the Zeeman interaction was used. The implementation of the mathematical model is presented in the LAMMPS software package, which was used to carry out numerical calculations. During the computational experiments, two separate problems were considered. In the first problem, the processes of deposition, interaction and ordering of a multilayer atomistic cobalt-iron-niobium system were analyzed. It has been shown that when niobium atoms are deposited onto a substrate, a relief nanofilm with irregularities up to a nanometer in height is formed. The contact between iron and niobium nanofilms is more blurred compared to the similar area of the contact between cobalt and iron nanofilms. In the second problem, the self-organization and reorientation of atomic spins in an iron nanofilm with a crystalline structure were analyzed. Calculations were carried out with and without an existing external magnetic field. The appearance of skyrmions (vortex flows) during the spin interaction of iron atoms was recorded. The simulation has shown that under the influence of an external magnetic field, an induced magnetic moment appears in the iron nanofilm, opposite to the induction vector of the external field.

Strain-driven skyrmion-bimeron switching in topological magnetic monolayer CrSeBr.

Skyrmion-bimeron switching is one of the most important phenomena in topological magnetism. Currently, it is usually realized by the annoying spin orientation vertical-reversal through magnetic field. Based on first-principles calculations and atomic spin simulations, we alternatively unveil that the switching between magnetic skyrmions and bimerons can be achieved in topological magnetic monolayer CrSeBr by external strain. The core mechanism of this switching is traced to the controllable magnetic anisotropy of monolayer CrSeBr influenced by the strain-engineered low-energy states around the Fermi level. We also introduce a parameter |κ| as a criterion for judging the stability of magnetic skyrmions and bimerons, which can be adopted as a useful descriptor linking the presence of skyrmion-bimeron switching driven by strain. The underlying physics is discussed in detail. The predicted strain controlled skyrmion-bimeron switching may be interesting for topological magnetic devices.

Expanding PyProcar for new features, maintainability, and reliability

This paper presents a comprehensive update to PyProcar, a versatile Python package for analyzing and visualizing density functional theory (DFT) calculations in materials science. The latest version introduces a modularized codebase, a centralized example data repository, and a robust testing framework, offering a more reliable, maintainable, and scalable platform. Expanded support for various DFT codes broadens its applicability across research environments. Enhanced documentation and an example gallery make the package more accessible to new and experienced users. Incorporating advanced features such as band unfolding, noncollinear calculations, and derivative calculations of band energies enriches its analytic capabilities, providing deeper insights into electronic and structural properties. The package also incorporates PyPoscar, a specialized toolkit for manipulating POSCAR files, broadening its utility in computational materials science. These advancements solidify PyProcar's position as a comprehensive and highly adaptable tool, effectively serving the evolving needs of the materials science community. New version program summaryProgram title: PyProcarCPC Library link to program files:https://doi.org/10.17632/d4rrfy3dy4.2Developer's repository link:https://github.com/romerogroup/pyprocarLicensing provisions: GPLv3Programming language: PythonSupplementary material: Pyprocar-Supplementary InformationJournal reference of previous version: Comput. Phys. Commun. 251 (2020) 107080, https://doi.org/10.1016/j.cpc.2019.107080Does the new version supersede the previous version?: YesReasons for the new version: Changes in the directory structure, the addition of new features, enhancement of the manual and user documentation, and generation of interfaces with other electronic structure packages.Summary of revisions: These updates enhance its capabilities and ensure developers' and users' maintainability, reliability, and ease of use.Nature of problem: To automate, simplify, and serialize the analysis of band structure and Fermi surface, especially for high throughput calculations.Solution method: Implement a Python library able to handle, combine, parse, extract, plot, and even repair data from density functional calculations from diverse electronic structure packages. PyProcar uses color maps on the band structures or Fermi surfaces to give a simple representation of the relevant characteristics of the electronic structure.Additional comments including restrictions and unusual features: PyProcar can produce high-quality figures of band structures and Fermi surfaces (2D and 3D), projection of atomic orbitals, atoms, and/or spin components.

Advancing magnetic material discovery through machine learning: Unveiling new manganese-based materials

Magnetic materials are used in a variety of applications, such as electric generators, speakers, hard drives, MRI machines, etc. Discovery of new magnetic materials with desirable properties is essential for advancement in these applications. In this research article, we describe the development and validation of a machine-learning model to discover new manganese-based stable magnetic materials. The machine learning model is trained on the input data from the Materials Project database to predict the magnetization and formation energy of the materials. New hypothetical structures are made using the substitution method, and the properties are predicted using the machine learning model to select the materials with desired properties. Harnessing the power of machine learning allows us to intelligently narrow down the vast pool of potential candidates. By doing so, we deftly reduce the number of materials that warrant in-depth examination using density functional theory, rendering the task more manageable and efficient. The selected materials, seemingly promising with their magnetic potential, undergo a meticulous validation process using the Vienna Ab initio Simulation Package, grounded in density functional theory. Our results underscore the paramount significance of input data in the efficacy of the machine learning model. Particularly in the realm of magnetic materials, the proper initialization of atomic magnetic spins holds the key to converging upon the true magnetic state of each material.

Characteristics of Tin Oxide Thin Film Grown by Atomic Layer Deposition and Spin Coating Process as Electron Transport Layer for Perovskite Solar Cells

Characteristics of Tin Oxide Thin Film Grown by Atomic Layer Deposition and Spin Coating Process as Electron Transport Layer for Perovskite Solar Cells

Hanle effect in transport through single atoms in spin-polarized STM

Following recent achievements in quantum-coherent manipulation and detection of individual atomic spins with the use of spin-polarized scanning tunneling microscope, we propose how to observe and utilize the Hanle effect in electronic transport in such setups. We show that the Hanle experiment can be used to observe the single spin precession driven by the intrinsic exchange field. This field is a result of virtual particle exchange processes, and its magnitude and sign can be controlled electrically. We also show that from detailed analysis of the Hanle resonance curve one can determine the spin relaxation time from dc current measurements.

Minimum separation between two pump pulses for ultrafast double magnetization switching in GdFeCo

Femtosecond laser ultrafast thermally induced magnetization switching (TIMS) has also attracted much attention due to its ability to trigger a single switching at the picosecond timescale. Current studies have shown that after a TIMS excited by a laser pulse, excitation of the switch again via TIMS does not require equilibrium between the subsystems. In this work, the main investigation is on the various possible cases of magnetization dynamics in GdFeCo under two short-delayed pulse excitations, as well as the factors limiting the minimum separation for double TIMS. These conditions are relevant for the potential application of TIMS to memory devices as it affects both the speed limit at which rewritten data is available and demonstrates the importance of spatial confinement of a laser pulse to bit size. The results show that low energy and short pulse duration lasers are prerequisites for double TIMS in GdFeCo based on simulations of atomic spin dynamics. By changing the damping constants of the alloy, we can shorten the minimum pulse separation between two pump pulses for double TIMS to 2 ps to approach terahertz frequency of write/erase cycles.

Acoustic frequency atomic spin oscillator in the quantum regime

Quantum noise reduction and entanglement-enhanced sensing in the acoustic frequency range is an outstanding challenge relevant for a number of applications including magnetometry and broadband noise reduction in gravitational wave detectors. Here we experimentally demonstrate quantum behavior of a macroscopic atomic spin oscillator in the acoustic frequency range. Quantum back-action of the spin measurement, ponderomotive squeezing of light, and virtual spring softening are observed at oscillation frequencies down to the sub-kHz range. Quantum noise sources characteristic of spin oscillators operating in the near-DC frequency range are identified and means for their mitigation are presented.

Manipulating the Spin Orientation of Co Atoms Using Monatomic Cu Chains.

Harnessing the spin of single atoms is at the heart of quantum information nanotechnology based on magnetic concepts. By attaching single Co atoms to monatomic Cu chains, we demonstrate the ability to control the spin orientation by the atomic environment. Due to spin-orbit coupling (SOC), the spin is tilted by ≈58° from the surface normal toward the chain as evidenced by inelastic tunneling spectroscopy. These findings are reproduced by density functional theory calculations and have implications for Co atoms on pristine Cu(111), which are believed to be Kondo systems. Our quantum Monte Carlo calculations suggest that SOC suppresses the Kondo effect of Co atoms at chains and on the flat surface. Our work impacts the fundamental understanding of low-energy excitations in nanostructures on surfaces and demonstrates the ability to manipulate atomic-scale magnetic moments, which can have tremendous implications for quantum devices.