Spin Coupling Research Articles

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.

Superconductivity in the pressurized nickelate La3Ni2O7 in the vicinity of a BEC–BCS crossover

Ever since the discovery of high-temperature superconductivity in cuprates, gaining microscopic insights into the nature of pairing in strongly correlated systems has remained one of the greatest challenges in modern condensed matter physics. Following recent experiments reporting superconductivity in the bilayer nickelate La3Ni2O7 (LNO) with remarkably high critical temperatures of Tc = 80 K, it has been argued that the low-energy physics of LNO can be described by the strongly correlated, mixed-dimensional bilayer t–J model. Here we investigate this bilayer system and utilize density matrix renormalization group techniques to establish a thorough understanding of the model and the magnetically induced pairing through comparison to the perturbative limit of dominating inter-layer spin couplings. In particular, this allows us to explain appearing finite-size effects, firmly establishing the existence of long-range superconducting order in the thermodynamic limit. By analyzing binding energies, we predict a BEC–BCS crossover as a function of the Hamiltonian parameters. We find large binding energies of the order of the inter-layer coupling that suggest strikingly high critical temperatures of the Berezinskii–Kosterlitz–Thouless transition, raising the question of whether (mixD) bilayer superconductors possibly facilitate critical temperatures above room temperature.

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.

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.

Disordered Heisenberg XYZ magnetic chains with exponential correlations: Localization and quantum state transfer

Our study investigates the Quantum State Transfer Protocol within a one-dimensional quantum Heisenberg spin chain model that features exponentially correlated disorder in the spin coupling distribution. We conducted extensive numerical simulations to explore how varying degrees of correlation impact the transfer of quantum states through this model of a quantum channel. Our results demonstrate that the extent of correlation significantly influences quantum communication along the channel. Specifically, we observed that in the strongly correlated regime, quantum communication remains largely unaffected even in large systems. These findings are interpreted in the context of the localization properties inherent to the disordered channel.

Halogen-Dependent Circular Dichroism and Magneto-Photoluminescence Effects in Chiral 2D Lead Halide Perovskites.

Chiral lead halide perovskites (chiral LHPs) have emerged as one of the best candidates for opto-spintronics due to their large spin-orbit coupling (SOC) and unique chirality-induced spin selectivity (CISS) even in the absence of a magnetic field. Here, we report the impact of halide composition on circular dichroism (CD) and magneto-photoluminescence (PL) effects of chiral 2D LHPs (R/S-MBA)2PbBrxI4-x (MBA = C6H5CH2(CH3)NH3). By tuning the mixing ratio of Br/I halide anions, we find that (R/S-MBA)2PbBrxI4-x thin films exhibit tunable and wide wavelength range CD signals. Simultaneously, the main CD signals near the exciton absorption band gradually blue shift until they disappear. Moreover, the halogen-dependent negative magneto-PL effects of (R/S-MBA)2PbBrxI4-x thin films excited by left/right circularly polarized light can be detected at room temperature. We demonstrated that the halide composition can effectively modulate exciton splitting and chirality transfer in (R/S-MBA)2PbBrxI4-x owing to the chirality-induced SOC and crystalline structure transition, which lead to the adjustable CD signals. The interplay of Rashba-type band spin splitting and spin mixing among bright triplet exciton states is responsible for the halogen-dependent magneto-PL effect of chiral 2D LHPs. This study enables chiral 2D LHPs with CISS to be a new class of promising opto-spintronics materials for exploring high-performance spin-light-emitting diodes by halide engineering.

4hJCHOCH Spin Coupling in a Lewisx Trisaccharide as Evidence of Inter-Residue C-H···O Hydrogen Bonding in Aqueous Solution.

Prior studies of the solution conformation of the Lewisx (Lex) trisaccharide, αFuc-(1→3)[βGal-(1→4)]-βGlcNAc, suggest that nonclassical inter-residue C-H···O hydrogen bonding in aqueous solution contributes to the stabilization of its 3D structure and affects its biological properties. Experimental evidence for this hydrogen bond in aqueous solution has been reported in the form of a 4hJCHOCH NMR spin-coupling constant between C5'Fuc and H1″Gal measured by 2D NMR methods in unlabeled samples. A methyl glycoside of Lex (MeβLex) was prepared containing selective 13C-labeling at C5'Fuc, and the H1″Gal signal was examined in high-field 1H NMR spectra for evidence of splitting or line-broadening caused by the 13C at C5'Fuc. High-resolution 1H NMR spectra obtained at high field and at different temperatures using different FID processing parameters showed no resolved splitting of the H1″Gal signal or evidence of line-broadening. Spectral simulation showed that this splitting and/or line-broadening would be observable if the reported J-value (∼1.1 Hz) is correct. DFT calculations on MeβLex and a carbon analog (O5″Gal replaced by a CH2 group) gave very small and nearly identical calculated 4hJC5',H1″ values, suggesting that the coupling is essentially zero. DFT calculations also showed that an alternate inter-residue 3hJH5',H1″ is small. Based on NMR analyses and DFT calculations, we found that 4hJC5',H1″ in MeβLex has an upper limit of ∼0.4 Hz and that the value could be lower, possibly zero, calling into question its value as experimental proof of persistent nonclassical hydrogen bonding in aqueous solutions of MeβLex and related structures.

DNA Catalysis: Design, Function, and Optimization.

Catalytic DNA has gained significant attention in recent decades as a highly efficient and tunable catalyst, thanks to its flexible structures, exceptional specificity, and ease of optimization. Despite being composed of just four monomers, DNA's complex conformational intricacies enable a wide range of nuanced functions, including scaffolding, electrocatalysis, enantioselectivity, and mechano-electro spin coupling. DNA catalysts, ranging from traditional DNAzymes to innovative DNAzyme hybrids, highlight the remarkable potential of DNA in catalysis. Recent advancements in spectroscopic techniques have deepened our mechanistic understanding of catalytic DNA, paving the way for rational structural optimization. This review will summarize the latest studies on the performance and optimization of traditional DNAzymes and provide an in-depth analysis of DNAzyme hybrid catalysts and their unique and promising properties.

Helium roaming in excess electrons in C60F60 as dynamic quasi-Matryoshka dolls.

Multi-guest clathrates exhibit lots of functional characteristics owing to their unique structures, which herald beautiful application prospects, but their fundamental information is still scarce. Herein, we explore a type of (helium, excess electrons/EEs)-C60F60 co-clathrates with quasi-Matryoshka-doll structures using abinitio molecular dynamics simulation and reveal the EEs-entangled He roaming dynamics in C60F60 and its effect on the characteristics of clathrates. Perfluorination ensures that C60F60 possesses an extremely electropositive interior cavity. Its unique confinement effect can stabilize He as an extremely inert entity by noticeably enlarging the 1s-2s orbital gap and can also trap 1-2 EEs in its s-type interior orbital with extremely large binding energies. Co-inclusion of He and EEs in C60F60 exhibits inter-repulsive He⋯EEs entangling dynamics featuring quasi-Matryoshka-doll structures (He@EEs@C60F60). In this structure, EEs screen the attraction of cage-shell Cδ+ to He 1s2 electrons, thus inhibiting their stabilization and orbital expansion, while He conversely decreases the stability of EEs and redshifts their transition absorption. He can roam in the cavity, but its trajectory is impacted by EEs serving as a medium, and thus, the structures exhibit anormal dynamic variation of internuclear He⋯C spin coupling JHeC, which is manipulated by the EEs-entangled He roaming dynamics. JHeC and JHeC' present opposite distance dependences for the colinearly aligned C⋅⋅⋅He⋅⋅⊗⋅⋅⋅⋅⋅C' (⊗, the cage center). This work provides insights into the Matryoshka-doll structured He@EEs@C60F60 with He-EEs entangling dynamics and its modulation on EEs absorption and reveals the dynamic role of EEs in manipulating He-roaming and JHeC coupling properties for promising applications.

Spin relaxation dynamics with a continuous spin environment: The dissipaton equation of motion approach.

We investigate the quantum dynamics of a spin coupling to a bath of independent spins via the dissipaton equation of motion (DEOM) approach. The bath, characterized by a continuous spectral density function, is composed of spins that are independent level systems described by the su(2) Lie algebra, representing an environment with a large magnitude of anharmonicity. Based on the previous work by Suarez and Silbey [J. Chem. Phys. 95, 9115 (1991)] and by Makri [J. Chem. Phys. 111, 6164 (1999)] that the spin bath can be mapped to a Gaussian environment under its linear response limit, we use the time-domain Prony fitting decomposition scheme to the bare-bath time correlation function (TCF) given by the bosonic fluctuation-dissipation theorem to generate the exponential decay basis (or pseudo modes) for DEOM construction. The accuracy and efficiency of this strategy have been explored by a variety of numerical results. We envision that this work provides new insights into extending the hierarchical equations of motion and DEOM approach to certain types of anharmonic environments with arbitrary TCF or spectral density.

XIAM-NQ: Implementation of exact quadrupole coupling

In rotational spectroscopy, the nuclear quadrupole coupling of spins to the rotation of a molecule frequently leads to significant hyperfine splittings of spectral lines, complicating spectral analysis. This complexity increases further when internal rotation fine splittings, particularly from methyl groups, are also present. The XIAM program, recognized in the community for its ability to address methyl internal rotation and handle nuclear quadrupole coupling for a single nucleus, while neglecting off-diagonal matrix elements in the quantum number J, has now been enhanced. The updated version, XIAM-NQ, includes the previously omitted matrix elements, enabling an exact treatment of quadrupole coupling. This new version offers precise spectral fits with minimal fitting times, even for molecules containing bromine and iodine nuclei. The effectiveness of XIAM-NQ is demonstrated on o-halotoluenes and m-chlorotoluene.

Direct Detection of the Magnetic Force and Field Coupling of Electronic Spins Using Photoinduced Magnetic Force Microscopy.

The intrinsic spin of the electron and its associated magnetic moment can provide insights into spintronics. However, the interaction is extremely weak, as is the case with the coupling between an electron's spin and a magnetic field, and it poses significant experimental challenges. Here we demonstrate the direct measurement of polarized single NV- centers and their spin-spin coupling behaviors in diamond. By using photoinduced magnetic force microscopy, we obtain the extremely weak magnetic force coupling originating from the electron spin. The polarized spin state of NV- centers, transitioning from |0⟩ to |±1⟩, and their corresponding Zeeman effect can be characterized through their interaction with a magnetic tip. The result presents an advancement in achieving electron spin measurements by magnetic force, avoiding the need for manufacturing conductive substrates. This facilitates a better understanding and control of electron spin to novel electronic states for future quantum technologies.

Four-step electron transfer coupled spin transition in a cyano-bridged [Fe2Co2] square complex.

The design of molecular functional materials with multi-step magnetic transitions has attracted considerable attention. However, the development of such materials is still infrequent and challenging. Here, a cyano-bridged square Prussian blue complex that exhibits a thermally induced four-step electron transfer coupled spin transition (ETCST) is reported. The magnetic and spectroscopic analyses confirm this multi-step transition. Variable-temperature infrared spectrum suggested the electronic structures in each phase and a four-step transition model is proposed.

Dragging of the particle spin and spin–spin coupling effect on its periapsis shift

Abstract The periapsis shift (PS) of spinning test particles in the equatorial plane of an arbitrary stationary and axisymmetric spacetime is studied using the post-Newtonian method. The result is expressed as a half-integer power series of $M/p$, where $M$ is the spacetime mass and $p$ is the semilatus rectum. The coefficients of the series are polynomials of the particle spin, the asymptotic expansion coefficients of the metric functions, and the eccentricity of the orbit. The particle spin is shown to have a similar effect as the Lense-Thirring (LT) effect on the PS, and both of them appear from the $(M/p)^{-3/2}$ order in the PS. The coupling between the spacetime and particle spins will increase (or decrease) the PS if they are parallel (or antiparallel). For Jupiter and Saturn rotating around the Sun and exceptionally designed satellites around Mercury and Moon, and the space-based gravitational wave observatories LISA and TaiJi around the Sun, the particle spin effect can be comparable to or even larger than the LT one in size. The PS in other spacetime studied are is not distinguishable from that in the Kerr spacetime to the $(M/p)^{-3/2}$ order.

Effective light-induced Hamiltonian for atoms with large nuclear spin

Ultracold fermionic atoms, having two valence electrons, exhibit a distinctive internal state structure, wherein the nuclear spin becomes decoupled from the electronic degrees of freedom in the ground electronic state. Consequently, the nuclear spin states are well isolated from the environment, rendering these atomic systems an opportune platform for quantum computation and quantum simulations. Coupling with off-resonance light is an essential tool to selectively and coherently manipulate the nuclear spin states. In this paper, we present a systematic derivation of the effective Hamiltonian for the nuclear spin states of ultracold fermionic atoms due to such an off-resonance light. We obtain compact expressions for the scalar, vector, and tensor light shifts taking into account both linear and quadratic contributions to the hyperfine splitting. The analysis has been carried out using the Green operator approach and solving the corresponding Dyson equation. Finally, we analyze different scenarios of light configurations which lead to the vector- and tensor-light shifts, as well as the pure spin-orbit coupling for the nuclear spin. Published by the American Physical Society 2024

Anomalous hybridized excitons induced by combined effects of Van der Waals coupling and Rashba spin–orbit coupling

As a typical transition-metal dichalcogenide, MoS2has drawn wide attention due to its good stability and excellent physicochemical properties, making it suitable for visible-region optoelectronic devices. To expand its application, bandgap engineering via heterostructure, thus far, was conventionally employed to tune the band gap. However, this strategy has the disadvantage that energy levels of bands do not show obvious changes compared to the isolated components, limiting the range of applications. Here, we achieve hybridized excitons induced by combined effects of Van der Waals (vdW) coupling and Rashba spin-orbit coupling (SOC), with a small exciton energy of 0.65 eV. For this purpose, we design a MoS2/MoWC heterostructure, where a built-in field (due to the absence of mirror symmetry) induces the Rashba SOC and contributes to the anomalous hybridized states, combined with the vdW coupling. An effective model is proposed to demonstrate the anomalous hybridized states for the heterostructure. Our approach reveals a novel mechanics model for hybridized excitons states, providing new physical ways to achieve infrared-region devices.

Discovering Classical Spin Liquids by Topological Search of High Symmetry Nets.

Spin liquids are a paradigmatic example of a nontrivial state of matter. The search for new spin liquids is a key interdisciplinary challenge. Geometrical frustration-where the geometry of the net that the spins occupy precludes the generation of a simple ordered state-is a particularly fruitful way to generate these intrinsically disordered states. Prior focus has been on a handful of high symmetry nets. There are, however, many three-dimensional nets, each of which has the potential to form unique states. In this paper, we investigate the high symmetry nets-those which are both vertex- and edge-transitive-for the simplest possible interaction sets: nearest-neighbor couplings of antiferromagnetic Heisenberg and Ising spins. While the well-known crs (pyrochlore) net is the only nearest-neighbor Heisenberg antiferromagnet which does not order, we identify two new frustrated nets (lcx and thp) possessing finite temperature Heisenberg spin-liquid states with strongly suppressed magnetic ordering and noncollinear ground states. With Ising spins, we identify three new classical spin liquids that do not order down to T/J = 0.01. We highlight materials that contain these high symmetry nets, and which could, if substituted with appropriate magnetic ions, potentially host these unusual states. Our systematic survey will guide searches for novel magnetic phases.

Nature of electrically detected magnetic resonance in highly nitrogen-doped 6H -SiC single crystals

This work focuses on unraveling electron paramagnetic resonance (EPR) and electrically detected magnetic resonance (EDMR) properties of n-type 6H silicon carbide (SiC) single crystals with high concentrations of uncompensated nitrogen (N) donors, which is essential for fundamental understanding of spin-related phenomena, developing spin-based devices, optimizing materials and devices, and advancing research in quantum information and spintronics. Utilizing low-temperature multifrequency EPR spectroscopy (9.4–395.12 GHz), we identified two intense signals labeled as S line and S1 line in the 6H-SiC crystals with ND–NA≈8×1018 and 4×1019cm−3. In addition, in 6H-SiC crystals with ND–NA≈8×1018cm−3, a low-intensity triplet from N donors substituting the quasicubic “k2” nonequivalent position (Nk2) was observed. The S line [g⊥=2.0029(2),g∥=2.0038(2)] was assigned to the exchange interaction of conduction electrons and Nk2, while the S1 line [g⊥=2.0030(2),g∥=2.0040(2)] is caused by the exchange spin coupling of localized N donors at the “k1” and “k2” positions. The S1 line was observed in high-frequency EDMR spectra of 6H-SiC with ND–NA≈8×1018cm−3, and its emergence was explained by an enhancement of the hopping conductivity due to the EPR-induced temperature increase mechanism. No EDMR spectra were found to occur in the 6H-SiC crystals with ND–NA≈4×1019cm−3, which is close to the critical donor concentration value for a semiconductor-metal transition. Thus it can be concluded that this N donor concentration is too high for the appearance of spin-dependent scattering and too low for the emergence of EPR-induced hopping mechanisms in 6H-SiC. Published by the American Physical Society 2024

Manipulation of anisotropic Zhang-Rice exciton in NiPS3 by magnetic field

The effect of external magnetic fields on the behavior of the Zhang-Rice exciton in NiPS3, which captures the physics of spin-orbital entanglement in 2D XY-type antiferromagnets, remains unclear. This study presents systematic study of angle-resolved and polarization-resolved magneto-optical photoluminescence spectra of NiPS3 in the Voigt geometry. We observed highly anisotropic, non-linear Zeeman splitting and polarization rotation of the Zhang-Rice exciton, which depends on the direction and intensity of the magnetic field and can be attributed to the spin-orbital coupling and field-induced spin reorientation. Furthermore, above the critical magnetic field, we detected additional splitting of the exciton peaks, indicating the coexistence of various orientations of Néel vector. This study characterizes orbital change of Zhang-Rice exciton and field-induced spin-reorientation phase transitions in a 2D hexagonal XY-type antiferromagnet, and it further demonstrates the continuous manipulation of the spin and polarization of the Zhang-Rice exciton.

Magnon excitation-induced spin memory loss in epitaxial L10-FePt/MgO/L10-FePt magnetic tunnel junctions

This work investigates the interplay between interfacial spin–orbit coupling (SOC) and magnon excitation-induced spin memory loss in epitaxial L10-FePt/MgO/L10-FePt magnetic tunnel junctions, which is crucial for advancing spintronic technologies. By employing systematic temperature-dependent transport measurements and inelastic electron tunneling spectroscopy, our study reveals that interfacial SOC at the Pt-terminated FePt/MgO interface significantly enhances magnon excitation during electron tunneling. This process results in a pronounced loss of spin memory in the spin-polarized current, diminishing the tunnel magnetoresistance ratio. Our findings provide critical insights into the mechanisms of spin memory loss, offering directions for optimizing spintronic device performance in the context of pronounced SOC environments.