Spin-orbit Coupling Research Articles

Large magnetocrystalline anisotropic energy and its impact on magnetostriction of L10-FePt

Abstract The origin of magnetocrystalline anisotropic energy (MAE) guided by spin–orbit coupling in the L10-FePt alloy was analyzed. Correlation of MAE with the calculated magnetoelastic constants in the single and polycrystal model was determined by means of first-principles calculations using density functional theory (DFT). More specifically, a systematic analysis of the large MAE and magnetostriction coefficients (λ’s) were done by means of post-processing of eigenvalues (orbital energies) and eigenfunctions (orbital occupancies). Our numerical analysis includes the convolution of the projected wave-function (density of states) of each orbital of the Fe and Pt sub-lattices into their orbital energies, which in principle should be valid for any solid regardless of the strength of the MAE. The determined anisotropic magnetostriction coefficients are of the λ ∼ 10 − 4 –10–3 order for several crystallographic directions; which is in accord to the known experimental data. However, the polycrystalline model based on the uniform stress approximation leads to a decrease of the λ by two orders in the overall magnetostrictive behavior ( λ ∼ 10 − 5 ). Such a large difference is not unexpected as the magnetostriction for polycrystalline FePt thin films were recorded as very low, thus validating the robustness of the current theoretical proposition of analyzing MAE.

Angular momentum properties of a circularly polarized vortex beam in the paraxial optical systems

The angular momentum (AM) properties of circularly polarized vortex beams (CPVBs) in two paraxial optical systems [free space and a gradient-index (GRIN) fiber] are demonstrated. The transverse light intensity, the longitudinal light intensity, the phase of the longitudinal electric field, the kinetic momentum, the total spin AM (SAM), the transverse-type SAM (t-SAM), the longitudinal-type SAM (l-SAM), and the orbital angular momentum (OAM) of CPVBs in the two paraxial optical systems are characterized. Spin-orbit coupling of CPVBs is studied during propagation in free space and in a GRIN fiber. When the OAM and the SAM of a CPVB have the same direction of rotation and when they have opposite directions of rotation, the spin-orbit coupling exhibits different characteristics in free space and in the GRIN fiber.

Spontaneous Magnetization Induced by Antiferromagnetic Toroidal Ordering

The magnetic toroidal dipole moment, which is induced by a vortex-type spin texture, manifests itself in parity-breaking physical phenomena, such as a linear magnetoelectric effect and nonreciprocal transport. We elucidate that a staggered alignment of the magnetic toroidal dipole can give rise to spontaneous magnetization even under antiferromagnetic structures. We demonstrate the emergence of uniform magnetization by considering the collinear antiferromagnetic structure with the staggered magnetic toroidal dipole moment on a bilayer zigzag chain. Based on the model calculations, we show that the interplay between the collinear antiferromagnetic mean field and relativistic spin-orbit coupling plays an important role in inducing the magnetization.

Topological signatures of triply degenerate fermions in Heusler alloys: an ab initio study

Triply degenerate nodal point (TP) fermions, lacking elementary particle counterparts, have been theoretically anticipated as quasiparticle excitations near specific band crossing points constrained by distinct space-group symmetries instead of Lorentz invariance. Here, based onfirst-principlescalculations and symmetry analysis, we demonstrate the presence of TP fermions in Heusler alloys. Furthermore, we predict that these Heusler alloys are dynamically stable, exhibiting TP fermions along four distinctC3axes in the F-43m space group. We show thatα-LiCaPdSb harbours peculiar Fermi arcs and surface states on the (111) and (001) crystal facets, owing to the coexistence of threefold rotational and time reversal symmetry. More interestingly, a modest tensile strain can increase the distance of fermions along the Γ-Lhigh symmetric line by as much as 21.10%, which give rise to measurable Fermi arcs. Furthermore, we investigate non-trivial topological insulator phase inβ-LiCaPdSb, by changing the chemical environment through placing transition metal atoms at various Wyckoff positions. Theβ-LiCaPdSb harbour a semi-metallic nature, and by breaking cubic symmetry, it undergoes a transition from semi-metal to a non-trivial topological insulator. In addition, for the first time, rare-earth LaPtBi half-Heusler alloy is examined under strain to uncover multiple band inversions associated with the TP fermionic phase. The observed multiple band inversion is entirely unaffected by spin-orbit coupling. We show that the LaPtBi compound hosts TP fermions, which are linked to aZ2topological invariant. Remarkably, with clear band crossings and multiple band inversion, we point out the possibilities of the LaPtBi for displaying a rich topological phase diagram. Our work provides a prototype material platform for experimental detection through angle-resolved photoemission spectroscopy or scanning tunnelling spectroscopy and practical spintronic applications.

What Can CISS Teach Us about Electron Transfer?

Electron transfer (eT) processes have garnered the attention of chemists and physicists for more than seven decades, and it is commonly believed that the essential features of the electron transfer mechanism are well understood─despite some open questions relating to the efficiency of long-range eT in some systems and temperature effects that are difficult to reconcile with the existing theories. The chiral induced spin selectivity (CISS) effect, which has been studied experimentally since 1999, demonstrates that eT through chiral systems depends on the electron's spin. Attempts to explain the CISS effect by adding spin-orbit coupling to the existing eT theories fails to reproduce the experimental results quantitatively, and it has become evident that the theory for explaining CISS must consider electron-vibration and/or electron-electron interactions. In this Perspective we identify some features of the CISS effect that imply that we should reconsider and refine the Marcus-Levich-Jortner mechanistic description for eT processes, especially for nonlinear systems and in the case of long-range eT.

Spin-orbit proximity in MoS2/bilayer graphene heterostructures

Van der Waals heterostructures provide a versatile platform for tailoring electronic properties through the integration of two-dimensional materials. Among these combinations, the interaction between bilayer graphene and transition metal dichalcogenides (TMDs) stands out due to its potential for inducing spin–orbit coupling (SOC) in graphene. Future devices concepts require the understanding of the precise nature of SOC in TMD/bilayer graphene heterostructures and its influence on electronic transport phenomena. Here, we experimentally confirm the presence of two distinct types of SOC – Ising (ΔI = 1.55 meV) and Rashba (ΔR = 2.5 meV) – in bilayer graphene when interfaced with molybdenum disulfide. Furthermore, we reveal a non-monotonic trend in conductivity with respect to the electric displacement field at charge neutrality. This phenomenon is ascribed to the existence of single-particle gaps induced by the Ising SOC, which can be closed by a critical displacement field. Our findings also unveil sharp peaks in the magnetoconductivity around the critical displacement field, challenging existing theoretical models.

Magnetic triple Weyl semimetals that are robust against spin-orbit coupling

Magnetic triple Weyl semimetals that are robust against spin-orbit coupling

Observation of doping-induced spin–orbit coupling in gold cluster assembly to carrier-tuneable semiconductors and Schottky behaviors

The doping influenced carrier dynamics to maneuvering n-type to p-type semiconducting gold cluster assembly have been assessed. The resonance photoemission spectroscopic measurements corroborate an incremental rise in the density of states at the valence edge, the overlap of valence states due to doping, and the presence of distinct spin–orbit splitting and coupling in manganese-doping (Au7Mn) compared to gold clusters (Au8), originating from the relativistic effect resulted in a semiconducting property. The work function dependent current–voltage characteristics in metal–semiconductor configuration show Ohmic and Schottky behaviors assorting p-type carriers in Au7Mn in contrast to the n-type Au8 and are presenting an atomic cluster based fast electronic device.

Tunable Anomalous Hall Effect in Broken–Symmetry Integrated Perovskite/Brownmillerite Superlattices

AbstractThe anomalous Hall effect (AHE), a hallmark of broken time–reversal symmetry, serves as a powerful tool for probing magnetic states and elucidating complex spin–orbit interactions in transition metal oxides. It is reported here that the emergence of AHE signals and interfacial ferromagnetism is directly observed from broken–symmetry integrated perovskite PrCoO3 and brownmillerite SrCoO2.5 superlattices. Through the strategic combinations of these two complex oxide systems onto the substrates with tailored lattice parameters, squared AHE hysteresis loops with perpendicular magnetic anisotropy are found under compressive strain in the optimized superlattices, and the magnitude of the loops is more than three times greater compared to those under tensile strain. The manifestation of AHE in these superlattices is attributed to an extrinsic mechanism involving spin–polarized scattering of charge carriers, with the mismatched perovskite/brownmillerite interfaces acting as the primary scattering centers. These discoveries suggest a promising avenue for the development of artificial materials with controllable AHE properties.

Material Transfer and Contact Optimization in MoS2 Nanotube Devices

While the promise of clean and defect‐free nanotubes as quantum electronic devices is obvious, ranging from strong spin–orbit interaction to intrinsic superconductivity, device fabrication still poses considerable challenges. Deterministic transfer of transition metal dichalcogenide nanomaterials and transparent contacts to the nanomaterials are nowadays highly active topics of research, both with fundamental research and applications in mind. Contamination from transport agents as well as surface adsorbates and surface charges play a critical role for device performance. Many techniques have been proposed to address these topics for transition metal dichalcogenides in general. Herein, their usage for the transfer‐based fabrication of nanotube devices is analyzed. Further, different contact materials are compared in order to avoid the formation of a Schottky barrier.

Spin and orbital magnetic moments of UTe2 induced by the external magnetic field

Correlated band theory implemented as a combination of the relativistic density functional theory with exact diagonalization [DFT+U(ED)] of the Anderson impurity term with Coulomb repulsion U in the 5f shell is applied to the magnetic field polarized state of \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\hbox {UTe}_2$$\\end{document}. We demonstrate that the DFT+U(ED) approach provides a good agreement with very recent x-ray absorbtion near edge structure (XANES) and x-ray magnetic circular dichroism (XMCD) experiments. The branching ratio for the \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$M_{4,5}$$\\end{document} edge transitions of uranium, and the valence spin-orbit interaction per hole were evaluated in a perfect agreement with the XANES. The orbital-to-spin moment ratio is calculated with DFT+U(ED) within the range of values extracted from XMCD data. The uranium atom 5f-shell ground state with 33 \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\%$$\\end{document} of \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$f^2$$\\end{document} and 58 \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\%$$\\end{document} of \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$f^3$$\\end{document} configurations is determined. Both XMCD and DFT+U(ED) point out the intermediate valence of uranium as well as itinerant-localized dichotomy in \\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$\\hbox {UTe}_2$$\\end{document}.

Spin-Lifetime Probe for Detecting Intramolecular Noncovalent Interaction in Organic Semiconductors.

Intramolecular noncovalent interaction (INCI), a crucial strategy for effectively enhancing molecular planarity and extending π-electron delocalization in organic semiconductors (OSCs), has played an increasingly important role in optoelectronic applications. However, though the INCI formation is regularly considered to improve the device performance by literature, there is no feasible approach to directly and reliably characterizing its formation in practical-OSC films thus far. Here in this study, by theoretical analysis and calculation, the generation of INCIs in OSCs is found, normally consisting of relatively heavy elements, such as O···Se, O···S, N···S interactions, etc., can induce enhanced strength of spin-orbit coupling, the primary factor dominating spin lifetime in OSCs. Based on this newly discovered theory, spin lifetime is creatively employed as a probe for sensitively detecting INCIs in OSC films via spin valves or field-induced electron paramagnetic resonance, respectively. This study will highly promote academic and applicable developments of the cross-cutting frontier research field between organic spintronics and electronics.

Significant enhancement in the magnetic properties of Cr2Te3 nanosheets by atom substitution doping.

Ferromagnetic Cr2Te3 nanocrystals, with their high spin-orbit coupling and low symmetry, have attracted considerable attention as rare-earth-free magnetic nanomaterials due to their potential to achieve high magnetic anisotropy. However, their relatively low values of remanence (Mr) and saturation (MS) magnetisation limit their energy product, making them unsuitable for practical applications. Herein, we report a straightforward one-pot heat-injection technique for the synthesis of high-remanence hexagonal Cr2Te3 nanosheets by heterogeneous doping with atoms of M (M = V, Mn and Se). The doped materials provide enhanced Mr and MS at an unchanged Curie temperature (TC), resulting in excellent hard magnetic properties. With Mn doping, the Mr of the matrix increases significantly, reaching 18.38 emu g-1 at 5 K, far exceeding the original undoped Cr2Te3 nanosheets. The nearly square hysteresis loop makes it valuable for many low temperature applications. These results provide a valuable case for tuning the magnetism of ferromagnetic Cr2Te3 by substitutional doping.

Exploration of lead free half-metallic double perovskites Li2Mo(Cl/Br)6 for spintronic device: DFT-calculations

The intrinsic spin of electrons has revolutionized the various aspects in the field of electronics, like data storage and quantum computing. Magnetic, structural, mechanical, transport and thermoelectric aspects of the Li2Mo(Cl/Br)6 double perovskites have been examined using the Wein2k and BoltzTraP code. These compounds having cubic structure with negative enthalpy of formation confirms their thermodynamic stability. The energy versus volume optimization for both ferromagnetic (FM) and antiferromagnetic phases (AFM) indicate AFM state due to greater release of energy in this configuration. Double exchange model p-d hybridization for partial density of states (PDOS) is investigated in band structures and half-metallicity feature is reported. The spin–orbit interaction with hybridization in d states of Mo and integral magnetic moment reveals strong spin polarization. The thermoelectric features (Seebeck coefficient, power factor, and figure of merit, electrical and thermal conductivities) have also been evaluated for utilization of these compounds in spintronics appliances.

Higher-order topological corner states and origin in monolayer LaBrO

Abstract Intrinsic higher-order topological insulators driven solely by orbital coupling are rare in electronic materials. Here, we propose that monolayer LaBrO is an intrinsic two-dimensional second-order topological insulator. The generalized second-order topological phase arises from the coupling between the 5d orbital of the La atom and the 2p orbital of the O atom. The underlying physics can be thoroughly described by a four-band generalized higher-order topological model. Notably, the edge states and corner states of monolayer LaBrO exhibit different characteristics in terms of morphology, number, and location distribution under different boundary and nanocluster configurations. Furthermore, the higher-order topological corner states of monolayer LaBrO are robust against variations in spin-orbit coupling and different values of Hubbard U. This provides a material platform for studying intrinsic 2D second-order topological insulators.

Consequences of the Pb-S Bond Formation for Lead Halide Perovskites.

Lead halide perovskites are structurally not stable due to their ionic bonds. Using sulfur agents in the crystal growth improves the stability and performance of the photovoltaic and light-emitting devices. In this theoretical work, we use a small toy S-radical in place of A cation in the bulk of lead iodide perovskite, and highlight the significance of the Pb-S covalent-double-bond formation for: the charge redistribution on the neighboring bonds that also turn to be covalent, phase transformation to a stable non-perovskite structure, and superior optoelectronic properties. The chemical analysis was performed with the Quantum Theory of Atoms In Molecules (QTAIM) and Non-Covalent Interactions (NCI) index. Excitonic properties were obtained from the solution of ab initio Bethe-Salpeter equation. Presence of the spin-orbit coupling triggers an interplay between the Frenkel and charge-transfer multiexcitons, switching between the photovoltaic and laser applications. Multiexcitons obey the exciton-fission preconditions.

Fractal surface states in three-dimensional topological quasicrystals

We study topological states of matter in quasicrystals, which do not rely on crystalline order. In the absence of a band-structure description and spin-orbit coupling, we show that a three-dimensional quasicrystal can nevertheless form a topological insulator. It relies on a combination of noncrystallographic rotational symmetry of quasicrystals and electronic orbital space symmetry, which is the quasicrystalline counterpart of the topological crystalline insulator. The resulting topological state obeys a nontrivial twisted bulk-boundary correspondence and lacks a good metallic surface. The topological surface states, localized on the top and bottom planes respecting the quasicrystalline symmetry, exhibit a different kind of multifractality with probability density concentrated mostly on high-symmetry patches. They form a near-degenerate manifold of immobile states whose number scales proportionally to the macroscopic sample size. This can present an opportunity for a platform for topological surface physics distinct from the crystalline counterpart. Published by the American Physical Society 2024

Two-dimensional BiSbTeX2 (X = S, Se, Te) and their Janus monolayers as efficient thermoelectric materials.

Today, there is a huge need for highly efficient and sustainable energy resources to tackle environmental degradation and energy crisis. We have analyzed the electronic, mechanical and thermoelectric (TE) characteristics of two-dimensional (2D) BiSbTeX2 (X = S, Se and Te) and Janus BiSbTeXY (X/Y = S, Se and Te) monolayers by implementing first principles simulations. These monolayers' dynamic stability and thermal stability have been demonstrated through phonon dispersion spectra and ab initio molecular dynamics (AIMD) simulations, respectively. The band structure of these monolayers can be tuned by applying uniaxial and biaxial strains. The investigated lattice thermal conductivity (κl) for these monolayers lies between 0.23 and 0.37 W m-1 K-1 at 300 K. For a more precise calculation of the scattering rate, we implemented electron-phonon coupling (EPC) and spin-orbit coupling effects to calculate the transport properties. For p(n)-type carriers, the power factor of these monolayers is predicted to be as high as 2.08 × 10-3 W m-1 K-2 and (0.47 × 10-3 W m-1 K-2) at 300 K. The higher thermoelectric figure of merit (ZT) of p-type carriers at 300 K is obtained because of their very low value of κl and high power factor. Our theoretical investigation predicts that these monolayers can be potential candidates for fabricating highly efficient thermoelectric power generators.

Ultralong Room-Temperature Phosphorescence in Ca(II) Metal-Organic Frameworks Based on Nicotinic Acid Ligands.

In recent years, metal-organic framework (MOF) materials with long persistent luminescence (LPL) have inspired extensive attention and presented various applications in security systems, information anticounterfeiting, and biological imaging fields. However, obtaining LPL materials with ultralong lifetime remains challenging. Halogen atoms, as nonmetallic elements existing in the frameworks, can not only induce the heavy-atom effect, effectively enhancing spin-orbit coupling and promoting intersystem crossing (ISC) processes, but also suppress non-radiative transition of the triplet states through the intra- and intermolecular interactions. Specifically, fluorine atoms with the strongest electronegativity may form intermolecular aggregate interlockings through halogen-bonding interactions that restrict molecular motions and vibrations, thereby improving phosphorescent lifetime. With the aforementioned considerations, two distinct types of MOFs with/without fluorine atoms (namely, Ca-MOF and 5FCa-MOF) were synthesized. Notably, by introducing fluorine atoms into MOFs, fluorine-induced intermolecular aggregate interlockings effectively enhanced the phosphorescent lifetime of 5FCa-MOF exceeding 264 ms compared to that of Ca-MOF (103.94 ms). Remarkably, both MOFs displayed bright LPL to the naked eye after removal of the irradiation source, especially 5FCa-MOF which can last for about 2 s. By introducing fluorine atoms, 5FCa-MOF exhibits greatly enhanced ISC with a rate constant up to 4.1 × 106 s-1 and suppressed non-radiative decay down to 3.73 s-1, thereby extending the LPL time. The thus obtained LPL provides potential in information encryption, security systems, optical anticounterfeiting, and so on.

Competing excitation quenching and charge exchange in ultracold Li-Ba+ collisions

Abstract Hybrid atom-ion systems are a rich and powerful platform for studying chemical reactions, as they feature both excellent control over the electronic state preparation and readout as well as a versatile tunability over the scattering energy, ranging from the few-partial wave regime to the quantum regime. In this work, we make use of these excellent control knobs, and present a joint experimental and theoretical study of the collisions of a single 138Ba+ ion prepared in the 5d 2D3/2,5/2 metastable states with a ground state 6Li gas near quantum degeneracy. We show that in contrast to previously reported atom-ion mixtures, several non-radiative processes, including charge exchange, excitation exchange and quenching, compete with each other due to the inherent complexity of the ion-atom molecular structure. We present a full quantum model based on high-level electronic structure calculations involving spin-orbit couplings. Results are in excellent agreement with observations, highlighting the strong coupling between the internal angular momenta and the mechanical rotation of the colliding pair, which is relevant in any other hybrid system composed of an alkali-metal atom and an alkaline-earth ion.