Spin Dynamics Research Articles

Creating Spin Channels in SrCoO3 through Trigonal‐to‐Cubic Structural Transformation for Enhanced Oxygen Evolution/Reduction Reactions

AbstractOxygen evolution and reduction reactions (OER and ORR) play crucial roles in energy conversion processes such as water splitting and air batteries, where spin dynamics inherently influence their efficiency. However, the specific contribution of spin has yet to be fully understood. In this study, we intentionally introduce a spin channel through the transformation of trigonal antiferromagnetic SrCoO2.5 into cubic ferromagnetic SrCoO3, aiming to deepen our understanding of spin dynamics in catalytic reactions. Based on the results from spherical‐aberration‐corrected microscopy, synchrotron absorption spectra, magnetic characterizations, and density functional theory calculations, it is revealed that surface electron transfer is predominantly governed by local geometric structures, while the presence of the spin channel significantly enhances the bulk transport of spin‐polarized electrons, particularly under high current densities where surface electron transfer is no longer the limiting factor. The overpotential for OER is reduced by at least 70 mV at 150 mA cm−2 due to the enhanced conductivity from spin‐polarized electrons facilitated by spin channels, with an expectation of even more significant reductions at higher current densities. This work provides a clearer picture of the role of spin in oxygen‐involved electrocatalysis, providing critical insights for the design of more efficient catalytic systems in practical applications.

Creating Spin Channels in SrCoO3 through Trigonal-to-Cubic Structural Transformation for Enhanced Oxygen Evolution/Reduction Reactions.

Oxygen evolution and reduction reactions (OER and ORR) play crucial roles in energy conversion processes such as water splitting and air batteries, where spin dynamics inherently influence their efficiency. However, the specific contribution of spin has yet to be fully understood. In this study, we intentionally introduce a spin channel through the transformation of trigonal antiferromagnetic SrCoO2.5 into cubic ferromagnetic SrCoO3, aiming to deepen our understanding of spin dynamics in catalytic reactions. Based on the results from spherical-aberration-corrected microscopy, synchrotron absorption spectra, magnetic characterizations, and density functional theory calculations, it is revealed that surface electron transfer is predominantly governed by local geometric structures, while the presence of the spin channel significantly enhances the bulk transport of spin-polarized electrons, particularly under high current densities where surface electron transfer is no longer the limiting factor. The overpotential for OER is reduced by at least 70 mV at 150 mA cm-2 due to the enhanced conductivity from spin-polarized electrons facilitated by spin channels, with an expectation of even more significant reductions at higher current densities. This work provides a clearer picture of the role of spin in oxygen-involved electrocatalysis, providing critical insights for the design of more efficient catalytic systems in practical applications.

Characterization of low sodium type II silicon clathrate film spin dynamics

Type II Si clathrate is a Si-based, crystalline alternative to diamond silicon with interesting optoelectronic properties. Here, a pulsed electron paramagnetic resonance study of the spin dynamics of sodium-doped, type II NaxSi136 silicon clathrate films is reported. Focusing on the hyperfine lines of isolated Na atoms, the temperature dependence of the electron spin dynamics is examined from 6 to 25 K. The measurements exhibit multi-exponential decay, indicating multiple spin relaxation rates in the system. As expected, spin relaxation time (T1) increases rapidly with decreasing temperature, reaching ∼300 μs at 6.4 K. The phase memory (TM) shows less temperature dependence with a value of ∼3 μs at the same temperature. The temperature dependence of T1 exhibits Arrhenius behavior in the measurement range consistent with an Orbach pathway. There are strong similarities to the spin behavior of other defect donors in diamond silicon. The results provide insights into the potential of Si clathrates for spin-based applications.

An explicitly magnetic modified embedded atom method formalism for coupled spin dynamics and molecular dynamics

Abstract In this paper, we augment the modified embedded atom method formalism to include magnetic spin-spin interactions for elements with a persistent magnetic moment. While previous spin coupling methods have been based on pair potentials, our Magnetic MEAM formalism, which we term MagMEAM, incorporates the many-body and angular effects of MEAM allowing for the strength of the magnetic interaction to vary with atomic environment. In particular, this allows potentials using this formalism to differentiate the magnetic interaction of different stable phases of magnetic elements such as the ferritic and austenitic phases of iron. This, in turn, allows for a more robust and realistic description of magnetism in polymorphic materials than was previously possible. The motivation for MagMEAM, including the insufficiency of magnetic pair potentials, is presented and the structure of the formalism is developed. A sample iron potential is developed using this formalism and shown to exceed the capabilities of existing magnetic pair potentials by simultaneously reproducing the magnetic energy of both martensite and austenite as well as the dynamic mechanical and magnetic properties of martensite. This newly designed formalism will allow for deeper explorations in the the complex interaction between different phases of polymorphic magnetic materials at the molecular dynamics scale.

Suppressing Energy Migration via Antiparallel Spin Alignment in One-Dimensional Mn2+ Halide Magnets with High Luminescence Efficiency.

Photoexcited energy migration is prone to causing luminescence quenching in Mn2+ luminescent materials, presenting a formidable challenge for optoelectronic applications. Although various strategies and mechanisms have been proposed to mitigate this issue, the role of spin alignment between adjacent Mn2+ ions has remained largely unexamined. In this study, we have elucidated the influence of spin alignment on energy migration within the one-dimensional Mn2+-metal halide compound (CH3)4NMnCl3 (TMMC) through variable-temperature photoluminescence (PL) and magnetic-optical spectroscopy. This investigation was conducted with reference to (CH6N3)2MnCl4 (GUA) with isolated [Mn3Cl12]6- trimers and Cd2+-doped TMMC. The spin order in TMMC below approximately 55 K is demonstrated by the disorder-order transition observed in the temperature-dependent magnetic susceptibility. This finding is further corroborated by the negligible shift in the temperature- and field-dependent emission peaks, a consequence of magnetic saturation. Our results indicate that the antiparallel spin alignment along the Mn2+ chain in TMMC effectively suppresses energy migration and multiphonon relaxation, thereby reducing nonradiative transitions and enhancing the photoluminescence quantum yield (PLQY). This research casts new light on the potential for developing high-performance Mn2+-doped phosphors for optoelectronic and spin-photonic applications, offering insights into the manipulation of spin and energy dynamics in these materials.

Effective spin dynamics of spin-orbit coupled matter-wave solitons in optical lattices

We consider matter–wave solitons in spin–orbit coupled Bose–Einstein condensates embedded in an optical lattice and study the dynamics of the soliton within the framework of Gross–Pitaevskii equations. We express spin components of the soliton pair in terms of nonlinear Bloch equations and investigate the effective spin dynamics. It is seen that the effective magnetic field that appears in the Bloch equation is affected by optical lattices, and thus the optical lattice influences the precessional frequency of the spin components. We make use of numerical approaches to investigate the dynamical behavior of density profiles and center-of-mass of the soliton pair in the presence of the optical lattice. It is shown that the spin density is periodically varying due to flipping of spinors between the two states. The amplitude of spin-flipping oscillation increases with lattice strength. We find that the system can also exhibit interesting nonlinear behavior for chosen values of parameters. We present a fixed point analysis to study the effects of optical lattices on the nonlinear dynamics of the spin components. It is seen that the optical lattice can act as a control parameter to change the dynamical behavior of the spin components from periodic to chaotic.

Spin-Hall conductivity and optical characteristics of noncentrosymmetric quantum spin Hall insulators: the case of PbBiI

Quantum spin Hall insulators have attracted significant attention in recent years. Understanding the optical properties and spin Hall effect in these materials is crucial for technological advancements. In this study, we present theoretical analyses to explore the optical properties, Berry curvature and spin Hall conductivity of pristine and perturbed PbBiI using the linear combination of atomic orbitals and the Kubo formula. The system is not centrosymmetric and it is hosting at the same time Rashba spin-splitting and quantized spin Hall conductivity. Our calculations reveal that the electronic structure can be modified using staggered exchange fields and electric fields, leading to changes in the optical properties. Additionally, the spin Berry curvature and spin Hall conductivity are investigated as a function of the energy and temperature. The results indicate that due to the small dynamical spin Hall conductivity, generating an ac spin current in the PbBiI requires the use of external magnetic fields or magnetic materials.

Dipolar Recoupling in Rotating Solids.

Magic angle spinning (MAS) nuclear magnetic resonance (NMR) has evolved significantly over the past three decades and established itself as a vital tool for the structural analysis of biological macromolecules and materials. This review delves into the development and application of dipolar recoupling techniques in MAS NMR, which are crucial for obtaining detailed structural and dynamic information. We discuss a variety of homonuclear and heteronuclear recoupling methods which are essential for measuring spatial restraints and explain in detail the spin dynamics that these sequences generate. We also explore recent developments in high spinning frequency MAS, proton detection, and dynamic nuclear polarization, underscoring their importance in advancing biomolecular NMR. Our aim is to provide a comprehensive account of contemporary dipolar recoupling methods, their principles, and their application to structural biology and materials, highlighting significant contributions to the field and emerging techniques that enhance resolution and sensitivity in MAS NMR spectroscopy.

Dynamics of spin oscillation in double barrier synthetic antiferromagnet based magnetic tunnel junction in presence of spin-transfer torque

In this work, we have studied the spin dynamics of a synthetic antiferromagnet (AFM)/heavy metal/ferromagnet double barrier magnetic tunnel junction in the presence of Ruderman–Kittel–Kasuya–Yosida (RKKY) interaction, interfacial Dzyaloshinskii–Moriya (iDM) interaction, Néel field, and Spin–Orbit Coupling (SOC) with different Spin-Transfer Torque (STT). We employ the Landau–Lifshitz–Gilbert–Slonczewski equation to investigate the AFM dynamics of the proposed system. We found that the system exhibits a transition from regular to damped oscillations with the increase in strength of STT for systems with a weaker strength of iDM interaction than RKKY interaction while displaying sustained oscillations for systems having the same order of RKKY and iDM interactions. On the other hand, the systems with sufficiently strong iDM interaction strength exhibit self-similar but aperiodic patterns in the absence of the Néel field. In the presence of the Néel field, the RKKY interaction dominating systems exhibit chaotic oscillations for low STT but display sustained oscillations under moderate STT. Our results suggest that the decay time of oscillations can be controlled via SOC. The system can work as an oscillator for low SOC but displays non-linear characteristics with the rise in SOC for systems having weaker iDM interaction than RKKY interactions. In contrast, opposite characteristics are noticed for iDM interaction dominating systems. We found periodic oscillations under low external magnetic fields in RKKY interaction dominating systems. However, moderate fields are necessary for sustained oscillation in iDM interaction dominating systems. Moreover, the system exhibits saddle-node bifurcations and chaos under moderate Néel field and SOC with suitable RKKY and iDM interactions. In addition, our results indicate that the magnon lifetime can be enhanced by increasing the strength of iDM interaction for both optical and acoustic modes.

Singlet, triplet, and mixed all-to-all pairing states emerging from incoherent fermions

The electron-electron and electron-phonon coupling in complex materials can be more complicated than simple density-density interactions, involving intertwined dynamics of spin, charge, and spatial symmetries. This motivates studying universal models with complex interactions and whether BCS-type singlet pairing is still the “natural” fate of the system. To this end, we construct a Yukawa-SYK model with nonlocal couplings in both spin and charge channels. Furthermore, we provide for time-reversal-symmetry breaking dynamics by averaging over the Gaussian unitary ensemble rather than the orthogonal ensemble. We find that the ground state of the system can be an orbitally nonlocal superconducting state arising from incoherent fermions with no BCS-like analog. The superconductivity has an equal tendency to triplet and singlet pairing states separated by a non-Fermi liquid phase. We further study the fate of the system within the superconducting phase and find that the expected ground state, away from the critical point, is a mixed singlet/triplet state. Finally, we find that, while at Tc the triplet and singlet transitions are dual to one another, below Tc the duality is broken, with the triplet state more susceptible to orbital fluctuations just by its symmetry. Our results indicate that such fluctuation-induced mixed states may be an inherent feature of strongly correlated materials. Published by the American Physical Society 2024

Element-specific ultrafast lattice dynamics in FePt nanoparticles

Light–matter interaction at the nanoscale in magnetic alloys and heterostructures is a topic of intense research in view of potential applications in high-density magnetic recording. While the element-specific dynamics of electron spins is directly accessible to resonant x-ray pulses with femtosecond time structure, the possible element-specific atomic motion remains largely unexplored. We use ultrafast electron diffraction (UED) to probe the temporal evolution of lattice Bragg peaks of FePt nanoparticles embedded in a carbon matrix following excitation by an optical femtosecond laser pulse. The diffraction interference between Fe and Pt sublattices enables us to demonstrate that the Fe mean square vibration amplitudes are significantly larger that those of Pt as expected from their different atomic mass. Both are found to increase as energy is transferred from the laser-excited electrons to the lattice. Contrary to this intuitive behavior, we observe a laser-induced lattice expansion that is larger for Pt than for Fe atoms during the first picosecond after laser excitation. This effect points to the strain-wave driven lattice expansion with the longitudinal acoustic Pt motion dominating that of Fe.

Efficient Quantum of Mechanical Simulation of Diffusion-Weighted MRI

Modern magnetic resonance imaging (MRI) experiments require simultaneous spin and spatial dynamics treatment. This paper aims to demonstrate the possibility of simulating a large spin system for diffusion-weighted MRI experiments. The numerical simulation of diffusion MRI depends on Bloch-Torrey equations. The latter describe the behavior of spin systems under the influence of magnetic fields and diffusion processes. They are particularly relevant in magnetic resonance imaging (MRI) and nuclear magnetic resonance (NMR) studies. The equations deal with uncoupled (-1/2) spins associated with three-dimensional spatial dynamics represented by diffusion and flow. The proposed method recommends using an unopened Kronecker product for evolution generators to minimize the simulation time and reduce the occupied computer memory. Two and three-dimensional diffusion-weighted magnetic resonance imaging associated with four pairs of coupled spin systems were utilized to achieve the study’s goals. Utilizing four pairs of coupled spin systems in MRI simulation enhances accuracy and realism in modeling interactions between spins, leading to improved tissue characterization and diagnostic capabilities. The obtained results were impossible using previous simulation packages. The results of the study demonstrate that the Spinach library can simulate complex spin systems with significant spatial dynamics.

Resonant spin dynamics of 2D electrons with strong Rashba and Zeeman couplings

Two-dimensional (2D) systems enable enhancing and diversifying the spin–orbit coupling of carriers, a key factor for better charge-spin conversion efficiencies in modern spintronic devices. Increasing 2D spin interactions also modifies dynamical spin-dependent properties of 2D materials, enabling to display resonant phenomena. In this work we focus on dynamical properties of the charge-spin conversion and analyze the resonant spin dynamics of 2D electrons upon strong spin–orbit coupling and Zeeman spin splittings, possibly exceeding the inverse relaxation times of electrons. We derive resonant frequencies and relaxation rates from the Bloch kinetic equations and examine how the trajectories of spin susceptibility poles change with variations in spin splittings and the relaxation time, paying special attention to the interplay between competing Rashba and Zeeman effect.

Time-resolved photoelectron spectroscopy at surfaces

Light is still an important spectroscopic tool for investigating the electronic structure of surfaces. Time-resolved photoelectron spectroscopy has mainly been developed in the last 30 years. It is therefore not surprising that the topic was hardly mentioned in the last issue on “The first thirty years” of surface science. In the second thirty years, however, we have seen tremendous progress in the development of time-resolved photoelectron spectroscopy on surfaces. Femtosecond light pulses and advanced photoelectron detection schemes are increasingly being used to study the electronic structure and dynamics of occupied and unoccupied electronic states and dynamic processes such as the energy and momentum relaxation of electrons, charge transfer at interfaces and collective processes such as plasmonic excitation and optical field screening. Using spin- and time-resolved photoelectron spectroscopy, we were able to study ultrafast spin dynamics, electron-magnon scattering and spin structures in magnetic and topological materials. Light also provides photon energy as well as electric and magnetic fields that can influence molecular surface processes to steer surface photochemistry and hot-electron-driven catalysis. In addition, we can consider light as a chemical reagent that can alter the properties of matter by creating non-equilibrium states and ultrafast phase transitions in correlated materials through the coupling of electrons, phonons and spins. Electric fields have also been used to temporarily change the electronic structure. This opened up new methods and areas such as high harmonic generation, light wave electronics and attosecond physics. This overview certainly cannot cover all these interesting topics. But also as a testimony to the cohesion and constructive exchange in our ultrafast community, a number of colleagues have come together to share their expertise and views on the very vital field of dynamics at surfaces. Following the introduction, the interested reader will find a list of contributions and a brief summary in Section 1.3.

Paramagnetic susceptibility and spin correlation function of ferromagnetic metals in the critical region

We study paramagnetic characteristics of ferromagnetic metals near the Curie temperature TC using the dynamic spin fluctuation theory. In contrast with most first-principles calculations, our results for the uniform paramagnetic susceptibility show a clear deviation from the Curie–Weiss law. We demonstrate that the susceptibility and correlation radius have the power-law behavior at temperatures up to 1.1–1.15TC, which gives an estimate for the region of critical temperatures in metals. Our theoretical critical exponents for Fe, Co, and Ni are in reasonable agreement with the low-field susceptibility measurements and neutron scattering experiments.

Spin fluctuations and orbital-selective superconductivity in Ba2CuO4-y: A FLEX study

Abstract Recently discovered Ba2CuO4-y provides new perspectives to the study of high-temperature superconductivity. Whereas, little is known about the spin dynamics of this material. In this work, we employ the fluctuation exchange (FLEX) approximation within the framework of spin-fluctuation mediated superconductivity to examine the behavior of the spin fluctuations of a two-orbital Hubbard model for Ba2CuO4-y. Our calculations reveal an extraordinary spin resonance mode coupled to the superconducting state in the hole-underdoped regime. Furthermore, we confirm that the coupling between the electrons and this resonance mode can lead to a “dip”-like feature in the electronic spectrum as a feedback effect. In the hole-overdoped regime, by incorporating self energy into our calculations, we obtain orbital-dependent renormalizations and show how these self-energy effects can lead to the detailed gap structures and the orbital-selective superconductivity, which could not be obtained in a previous study using random phase approximation (RPA). This research may shed a new light on searching for unconventional superconductors with higher transition temperatures.

RadicalPy: A Tool for Spin Dynamics Simulations.

Radical pairs (electron-hole pairs, polaron pairs) are transient reaction intermediates that are found and exploited in all areas of science, from the hard realm of physics in the form of organic semiconductors, spintronics, quantum computing, and solar cells to the soft domain of chemistry and biology under the guise of chemical reactions in solution, biomimetic systems, and quantum biology. Quantitative analysis of radical pair phenomena has historically been successful by a few select groups. With this in mind, we present an intuitive open-source framework in the Python programming language that provides classical, semiclassical, and quantum simulation methodologies. A radical pair kinetic rate equation solver, Monte Carlo-based spin dephasing rate estimations, and molecule database functionalities are implemented. We introduce the kine-quantum method, a new approach that amalgamates classical rate equations, semiclassical, and quantum techniques. This method resolves the prohibitively large memory requirement issues of quantum approaches while achieving higher accuracy, and it also offers wavelength-resolved simulations, producing time- and wavelength-resolved magnetic field effect simulations. Model examples illustrate the versatility and ease of use of the software, including the new approach applied to the magnetosensitive absorption and fluorescence of flavin adenine dinucleotide photochemistry, spin-spin interaction estimation from molecular dynamics simulations on radical pairs inside reverse micelles, radical pair anisotropy inside proteins, and triplet exciton pairs in anthracene crystals. The intuitive interface also allows this software to be used as a teaching or learning aid for those interested in the field of spin chemistry. Furthermore, the software aims to be modular and extensible, with the aim to standardize how spin dynamics simulations are performed.

Unusual spin dynamics in the van der Waals antiferromagnet FeGa2S4

Spin dynamics in the van der Waals antiferromagnet FeGa2S4with triangular lattices are investigated using magnetometry, neutron scattering, and muon spin relaxation measurements. The characteristic spin relaxation time is thoroughly clarified over thirteen orders of magnitude. Although the temperature dependence of DC and AC susceptibilities recalls a conventional spin-glass transition, nonlinear susceptibilities showing no divergences at the anomalous temperature,T∗=16.87(7) K, deny that and instead hint at other mechanisms. Elastic neutron scattering together with previously measured muon results depict a slowly fluctuated (∼10-5 s) spin state aboveT∗. In juxtaposing the underlying simplest structure among frustrated magnets with an intricate hierarchy of time scales, FeGa2S4can be a playground for studying temporal spin correlations in the two-dimensional limit.

Nutation-orbit resonances: The origin of the chaotic rotation of Hyperion and the barrel instability

While numerous planetary and asteroid satellites show evidence for non-trivial rotation states, none are as emblematic as Hyperion, which has long been held as the most striking example of chaotic spin-orbit evolution in the Solar System. Nevertheless, an analytically tractable theory of the full 3D spin-orbit dynamics of Hyperion has not been developed. We derive the Hamiltonian for a spinning axisymmetric satellite in the gravitational potential of a planet without assuming planar or principal axis rotation and without averaging over the spin period. Using this model, we demonstrate the emergence of resonances between the nutation and orbital frequencies that act as the primary drivers of the spin dynamics. This analysis reveals that, contrary to long-held belief, Hyperion is not tumbling chaotically. Instead, it lies near or in a nutation-orbit resonance that is first-order in eccentricity, allowing it to rotate quasi-regularly. The most reliable observations are consistent with either nonchaotic motion or chaos that is orders of magnitude smaller than originally claimed. A separate phenomenon, the so-called barrel instability, is shown to be related to a different set of nutation-orbit resonances that generalize the planar spin-orbit resonances. Finally, we show that changes in spin states over long timescales are best understood by considering chaotic diffusion of quasi-conserved quantities.

Néel Vector Auto-Oscillations and Reorientations Induced by Spin-Polarized Electric Currents in Antiferromagnetic Mn2Au Nanolayer

The electrical excitation of spin dynamics in antiferromagnets is important for the development of high-speed spintronic devices with a low power consumption. Here, we present a theoretical study of the spin dynamics generated in the Ni/Cu/Mn2Au/Cu/Ni nanostructure by a perpendicular-to-plane electric current. Our investigation includes atomistic simulations of spin reorientations in a few monolayer antiferromagnetic Mn2Au film and numerical calculations of nonequilibrium spin accumulation in the nanostructure comprising ferromagnetic Ni polarizers with antiparallel magnetizations. This combined approach enables us to quantify the dynamics of Mn magnetic moments induced by the spin-transfer torque created by the spin-polarized charge flow. The calculations show that the direct electric current with the density exceeding some temperature-dependent threshold value gives rise to steady-state auto-oscillations of the Néel vector in the [Formula: see text]-oriented Mn2Au nanolayer. As the precession of Mn magnetic moments occurs around an out-of-plane direction strongly deflected from their initial in-plane orientations, the emergence of auto-oscillations should be regarded as the realization of a dynamic spin reorientation transition in the antiferromagnetic crystal. Remarkably, the precession frequency rises with increasing current density J and exceeds 1[Formula: see text]THz at [Formula: see text][Formula: see text]A[Formula: see text]m[Formula: see text], which makes the described antiferromagnetic spin transfer nano-oscillator attractive for device applications. Furthermore, our simulations demonstrate that a picosecond current pulse injected into the Ni/Cu/Mn2Au/Cu/Ni nanostructure can induce a precessional switching of the Néel vector. Depending on the current density and pulse duration, the Néel vector rotates by either 90° or 180° and attains stable orientation along the corresponding [Formula: see text] easy axis in the plane of the Mn2Au nanolayer. This feature shows that the Ni/Cu/Mn2Au/Cu/Ni nanostructure could be used as a nonvolatile memory cell with the electrical writing and readout.