Local Spin Research Articles

Chiral nanoparticle separation and discrimination using radially polarized circular Airy vortex beams with orbital-induced spin angular momentum.

We report orbit-induced localized spin angular momentum associated with optical spin-orbit interactions in tightly focused radially polarized circular Airy vortex beams and demonstrate their potential for separation and discrimination of chiral nanoparticles. We find that variations in spin angular momentum density endow these beams with positive and negative annular optical chirality density. Utilizing these extraordinary distributions, particles having different chirality parameters can be separated and discriminated by using two degrees of freedom, i.e., radial trapping position and azimuthal rotation. We also discuss the impacts of longitudinal optical force and topological charge on manipulating chiral particles. Additionally, we conduct a comparative analysis of the optical trapping of a non-chiral particle. Our work is expected to deepen the understanding of spin-orbit interactions and provide valuable insight into vortex beam interactions with chiral particles.

Hydrogen-designed spin-states of 2D silicon carbide and graphene nanostructures.

Identifying and manipulating spin in two-dimensional materials is of great interest in advancing quantum information and sensing technologies, as well as in the development of spintronic devices. Here, we investigate the influence of hydrogen adsorption on the electronic and magnetic properties of graphene-like triangulenes. We have constructed triangulenes from SiC monolayers, which have been successfully synthesized very recently, extending our investigation to include graphene triangulenes. This advancement in the synthesis of SiC monolayers allows us to investigate deeper into the unique properties of SiC-based triangulenes and compare them with their graphene counterparts. The addition of hydrogen has been found to induce a magnetic moment in the SiC monolayer, with a more localized spin density when H is adsorbed in the C sites while spreading through the lattice when adsorbed on the Si sites. In triangular flakes, the ground spin state changes with the adsorption site: decreasing multiplicity on edge-defined sublattices and increasing it on the opposite sublattice. These findings suggest hydrogen adsorption as a tool for tuning spin-state properties in SiC and graphene nanostructures, with potential applications in spintronics and spin quantum dot devices.

Doping effect on electronic and magnetic properties of Ag-doped single-walled (6,0) GaN nanotubes: First-principles study

The electronic and magnetic properties of GaN wurtzite, un-doped, and Ag-doped single-walled (6,0) chiral GaN nanotubes (SWGaNNT) were investigated using Density Functional Theory and Local Spin Density Approximation methods within Hubbard U semiempirical correction (DFT-LSDA + U). In a consecutive DFT-LSDA + U electronic structure simulation, the effects of defects on the nature and origin of ferromagnetism (FM) are studied for an Ag-doped SWGaNNT system. For the Ag-doped GaN nanotube configurations, the energy gap decreases with increasing concentration of impurity. The total energy calculations for doped systems show the stability of the ferromagnetic phase. In the case of the Ag-doping GaN NT system, the wide energy gap is decreasing and the total magnetic moment of this system is ∼2.0 μB. From first-principles calculations, an Ag-doped GaN nanosystem can be made into a magnetic ferromagnetic material, and it is an important candidate for spintronics device applications.

Structure, Spin Correlations, and Magnetism of the S = 1/2 Square-Lattice Antiferromagnet Sr2CuTe1-xWxO6 (0 ≤ x ≤ 1).

Quantum spin liquids are highly entangled magnetic states with exotic properties. The S = 1/2 square-lattice Heisenberg model is one of the foundational models in frustrated magnetism with a predicted, but never observed, quantum spin liquid state. Isostructural double perovskites Sr2CuTeO6 and Sr2CuWO6 are physical realizations of this model but have distinctly different types of magnetic order and interactions due to a d10/d0 effect. Long-range magnetic order is suppressed in the solid solution Sr2CuTe1-xWxO6 in a wide region of x = 0.05-0.6, where the ground state has been proposed to be a disorder-induced spin liquid. Here, we present a comprehensive neutron scattering study of this system. We show using polarized neutron scattering that the spin liquid-like x = 0.2 and x = 0.5 samples have distinctly different local spin correlations, which suggests that they have different ground states. Low-temperature neutron diffraction measurements of the magnetically ordered W-rich samples reveal magnetic phase separation, which suggests that the previously ignored interlayer coupling between the square planes plays a role in the suppression of magnetic order at x ≈ 0.6. These results highlight the complex magnetism of Sr2CuTe1-xWxO6 and hint at a new quantum critical point between 0.2 < x < 0.4.

Unveiling exotic magnetic phase diagram of a non-Heisenberg quasicrystal approximant

A magnetic phase diagram of the non-Heisenberg Tsai-type 1/1 Au-Ga-Tb approximant crystal (AC) has been established across a wide electron-per-atom (e/a) range via magnetization and powder neutron diffraction measurements. The diagram revealed exotic ferromagnetic (FM) and antiferromagnetic (AFM) orders that originate from the unique local spin icosahedron common to icosahedral quasicrystals (iQCs) and ACs; The noncoplanar whirling AFM order is stabilized as the ground state at the e/a of 1.72 or less whereas a noncoplanar whirling FM order was found at the larger e/a of 1.80, with magnetic moments tangential to the Tb icosahedron in both cases. Moreover, the FM/AFM phase selection rule was unveiled in terms of the nearest neighbour (J1) and next nearest neighbour (J2) interactions by numerical calculations on a non-Heisenberg single icosahedron. The present findings will pave the way for understanding the intriguing magnetic orders of not only non-Heisenberg FM/AFM ACs but also non-Heisenberg FM/AFM iQCs, the latter of which are yet to be discovered.

Inzhektsiya spina dvizhushcheysya domennoy stenkoy na granitse razdela antiferromagnitnogo izolyatora s dvumernym metallom

A domain wall (DW) which moves parallel to a magnetically compensated interface between an antiferromagnetic insulator (AFMI) and a two-dimensional (2D) metal can pump spin polarization into the metal. It is assumed that localized spins of a collinear AFMI interact with itinerant electrons through their exchange interaction on the interface. We employed the Keldysh formalism of Green’s functions for electrons which experience potential and spin-orbit scattering on random impurities. This formalism allows a unified analysis of spin pumping, spin diffusion and spin relaxation effects on a 2D electron gas. It is shown that the pumping of a nonstaggered magnetization into the metal film takes place in the second order with respect to the interface exchange interaction. At sufficiently weak spin relaxation this pumping effect can be much stronger than the first-order effect of the Pauli magnetism which is produced by the small nonstaggered exchange field of the DW. It is shown that the pumped polarization is sensitive to the geometry of the electron’s Fermi surface and increases when the wave vector of the staggered magnetization approaches the nesting vector of the Fermi surface. In a disordered diffusive electron gas the induced spin polarization follows the motion of the domain wall. It is distributed asymmetrically around the DW over a distance which can be much larger than the DW width.

The effect of composition on the structure, optical, and room-temperature ferromagnetic properties of hydrothermally synthesized (ZnSn)1-xCuxO nanocomposites

(ZnSn)1-xCuxO nanocomposites (NCs) with nanorods and nanosheet morphologies were synthesized by a facile hydrothermal technique. (ZnSn)1-xCuxO NCs exhibited a gradual band gap redshift from UV to visible spectral region with increasing Cu-content. The room temperature magnetic hysteresis loop indicated the improvement of room temperature ferromagnetic (RTFM) behavior of (ZnSn)1-xCuxO NCs compared with nanostructured ZnSnO NCs induced by the exchange interaction of Cu-bound polarons with the localized spins and free carriers. The (ZnSn)60Cu40O NCs exhibited the highest saturation magnetization (Ms) of 0.539 emu·g−1. Further increase in Cu-content resulted in the deterioration of crystalline domains and the reduction of Ms to 0.259 emu·g−1. This behavior revealed that the electronic and magnetic properties of (ZnSn)1-xCuxO NCs were so sensitive to the dopant concentration that need to be utilized for improving their performance as good candidate NCs for spintronic applications.

Large off-diagonal magnetoelectricity in a triangular Co2+-based collinear antiferromagnet

Magnetic toroidicity is an uncommon type of magnetic structure in solid-state materials. Here, we experimentally demonstrate that collinear spins in a material with R-3 lattice symmetry can host a significant magnetic toroidicity, even parallel to the ordered spins. Taking advantage of a single crystal sample of CoTe6O13 with an R-3 space group and a Co2+ triangular sublattice, temperature-dependent magnetic, thermodynamic, and neutron diffraction results reveal A-type antiferromagnetic order below 19.5 K, with magnetic point group -3′ and k = (0,0,0). Our symmetry analysis suggests that the missing mirror symmetry in the lattice could lead to the local spin canting for a toroidal moment along the c axis. Experimentally, we observe a large off-diagonal magnetoelectric coefficient of 41.2 ps/m that evidences the magnetic toroidicity. In addition, the paramagnetic state exhibits a large effective moment per Co2+, indicating that the magnetic moment in CoTe6O13 has a significant orbital contribution. CoTe6O13 embodies an excellent opportunity for the study of next-generation functional magnetoelectric materials.

On renormalization and the local gap method for proving frustration-free local spin chains are gapped

Key properties of a physical system depend on whether it is gapped, i.e., whether its spectral gap has a positive lower bound that is independent of system size. Here, we provide a prescription for renormalizing a spin chain Hamiltonian in such a way that the renormalized Hamiltonian is gapped if and only if the original Hamiltonian is gapped. Then, we articulate a set of conditions that guarantees the renormalized Hamiltonian is gapped. These conditions are built on a certain strong notion of decaying correlations involving an operator norm of non-commuting terms in the renormalized Hamiltonian. We apply the method to show that two interesting models, with forms motivated by quantum circuits, are gapped. We also confirm the generality of the method by successfully applying it to a somewhat different case, the well-known Affleck-Kennedy-Lieb-Tasaki (AKLT) model.

Altering the Localization of an Unpaired Spin in a Formal Ni(V) Species.

The participation of both ligand and the metal center in the redox events has been recognized as one of the ways to attain the formal high valent complexes for the late 3d metals, such as Ni and Cu. Such an approach has been employed successfully to stabilize a Ni(III) bisphenoxyl diradical species in which there exist an equilibrium between the ligand and the Ni localized resultant spin. The present work, however, broadens the scope of the previously reported three oxidized equivalent species by conveying the approaches that tend to affect the reported equilibrium in CH3 CN at 233 K. Various spectroscopic characterization revealed that employing exogenous N-donor ligands like 1-methyl imidazole and pyridine favors the formation of the Ni centered localized spin though axial binding. In contrast, due to its steric hinderance, quinoline favors an exclusive ligand localized radical species. DFT studies shed light on the novel intermediates' complex electronic structure. Further, the three oxidized equivalent species with the Ni centered spin was examined for its hydrogen atom abstraction ability stressing their key role in alike reactions.

First-principles prediction of higher Curie temperature, metallic and half-metallic ferromagnetism in Zn1-x(Vx,Nix)O systems

The electronic and magnetic properties of Zn(V,Ni)O systems with 2.08 %, 4.16 %, 6.25 %, 8.3 %, and 12.5 % impurity concentrations were investigated based on ab initio simulations. The first-principles calculations were carried out using density functional theory and local spin density approximation by pseudopotential method. Analyzing the calculated density of states, the mechanism to stabilize the ferromagnetic phase in the 3d-metals doped ZnO systems is discussed. The analysis of the total density of states shows that the V-doped ZnO presents a metallic nature and Ni-doped ZnO exhibits a half-metallic character. First-principles calculations show that the stability of ferromagnetic or antiferromagnetic behaviors depends on impurity concentrations and impurity positions in related ZnO:V,Ni systems. Finally, we estimated and studied the Curie temperatures for V- and Ni-doped ZnO systems with different impurity concentrations. The Curie temperatures for VxZn1-xO and NixZn1-xO systems are higher than room temperature and these compounds are suitable ferromagnetic DMS materials for spintronic applications.

Unveiling the Robust Struct-Electromagnetic Characteristics of CdAB2 Chalcopyrite (A = Cr, Mn, Fe; B = P, As): A Comprehensive Ab-Initio Study

We present a comprehensive investigation of the electromagnetic properties of CdAB2 compounds, where A represents Cr, Mn, or Fe, and B denotes P or As. To investigate the spin-polarized behavior of these compounds the A atoms were substituted at the Group IV (Ge) position in CdGeB2 in the chalcopyrite crystal structure. Our results reveal that all the CdAB2 compounds exhibit compelling spin-splitting of energy states near the Fermi level (EF). Notably, CdAB2 materials with A = Cr and Mn exhibit intriguing half-metallic ferromagnetic (HMF) characteristics, with the calculated total magnetic moments of 2.00 and 3.00 µB/f.u., respectively. The HMF properties originated in CdAB2 (A = Cr and Mn; B = P, As) these compounds owing to the hybridization of partially filled -3d(t2g) states of A atoms with the p-states of B (P, As) atoms, with minor contributions from Cd’s-like states. In contrast, CdFeB2 displays distinct behavior, demonstrating spin-splitting of energy levels around the EF indicative of a stable ferromagnetic (FM) state and the absence of HMF at their equilibrium volume. The calculated total magnetic moments for CdFeP2 and CdFeAs2 are about 1.83 (1.64 µB/f.u.) and 1.94 µB/f.u. (1.84 µB/f.u.) under generalized gradient approximation (GGA) (local spin density approximation (LSDA)) approximations, respectively. Perhaps these CdAB2 compounds (A = Cr and Mn; B = P, As) with HMF characteristic within both LSDA and GGA formalisms makes them highly promising candidates for spin injectors in the spintronic device applications. Furthermore, their semiconducting nature renders CdCrB2 and CdMnB2 materials compatible with silicon and other semiconducting lattices, enhancing their potential practical applications in the spintronic technologies. In conclusion, this study presents a thorough exploration of the robust electronic and magnetic properties of CdAB2 chalcopyrites, offering exciting prospects for their utilization in the future spintronic applications.

Superdiffusion from Nonabelian Symmetries in Nearly Integrable Systems

The Heisenberg spin chain is a canonical integrable model. As such, it features stable ballistically propagating quasiparticles, but spin transport is subballistic at any nonzero temperature: An initially localized spin fluctuation spreads in time t to a width t2/3. This exponent as well as the functional form of the dynamical spin correlation function suggest that spin transport is in the Kardar–Parisi–Zhang (KPZ) universality class. However, the full counting statistics of magnetization is manifestly incompatible with KPZ scaling. A simple two-mode hydrodynamic description, derivable from microscopic principles, captures both the KPZ scaling of the correlation function and the coarse features of the full counting statistics, but remains to be numerically validated. These results generalize to any integrable spin chain invariant under a continuous nonabelian symmetry and are surprisingly robust against moderately strong integrability-breaking perturbations that respect the nonabelian symmetry.

Theoretical studies on the local structure and spin Hamiltonian parameters for Cu2+ ions in LiTaO3 crystal.

The local structure and spin Hamiltonian parameters (SHPs) g factors (gx , gy , gz ) and the hyperfine structure constants (Ax , Ay , Az ) for Cu2+ doped in the LiTaO3 crystal are theoretically investigated by the perturbation formulas for a 3d9 ion under rhombically elongated octahedral based on the cluster approach. The impurity Cu2+ was assumed to occupy the host trigonally-distorted octahedral Li+ site and experience the Jahn-Teller (JT) distortion from the host trigonal octahedral [TaO6 ]10- to the impurity rhombically elongated octahedral [CuO6 ]10- . Based on the calculations, the impurity-ligand bond lengths parallel and perpendicular to the C2 -axis are found to be R|| (≈ 2.305 Å) and R⊥ (≈ 2.112 Å) for the studied [CuO6 ]10- cluster, with the planar bond angle θ (≈ 78.2°). Meanwhile, the ground-state wave function for Cu2+ center in LiTaO3 was also obtained. The calculated SHPs based on the above local lattice distortions agree well with the experimental data, and the results are discussed.

Ferrimagnetic charge order in molecular conductors with diluted localized spins exhibiting enhanced giant magnetoresistance effect

Ferrimagnetic charge order in molecular conductors with diluted localized spins exhibiting enhanced giant magnetoresistance effect

Jahn–Teller Magnets

A wide class of materials with different crystal and electronic structures including quasi-2D unconventional superconductors, such as cuprates, nickelates, ferropnictides/chalcogenides, ruthenate Sr2RuO4, and 3D systems, such as manganites RMnO3, ferrates (CaSr)FeO3, nickelates RNiO3, silver oxide AgO, are based on Jahn–Teller 3d and 4d ions. These unusual materials, called Jahn–Teller (JT) magnets, are characterized by an extremely rich variety of phase states, spanning from non-magnetic and magnetic insulators to unusual metallic and superconducting states. The unconventional properties of JT magnets can be attributed to the instability of their highly symmetric Jahn–Teller “progenitors” with the ground orbital E-state with repect to charge transfer, anti-Jahn–Teller d-d disproportionation, and the formation of a system of effective local composite spin–singlet or spin–triplet, electronic, or hole S-type bosons moving in a non-magnetic or magnetic lattice. We consider specific features of the anti-JT-disproportionation reaction, properties of the electron–hole dimers, possible phase states and effective Hamiltonians for single- and two-band JT magnets, concluding with a short overview of physical properties for actual JT magnets.

Electronic structure of SrFe1−x(Mn,Co)xO3-δ: A CPA case study

A new methodology is suggested for determining and using the Coulomb interaction parameter U(t2g), taking into account the different energy localizations of t2g and eg states in disordered transition metal perovskite-like oxides, based on the local spin density approximation with Coulomb interaction correction method and the coherent potential approximation. The adjustment of U(t2g)’s relies on the best coincidence of the experimental and calculated maxima in X-ray absorption/reflection spectra at simultaneous demand for the calculated magnetic moments to closely correspond to their experimental values in cubic oxides SrFeO3, SrMnO3, and SrCoO3. Then, the obtained U’s are utilized in order to construct the Green functions for calculating the electronic properties of strongly correlated perovskite-like solid solutions within the coherent potential method. The high efficiency of the proposed methodology has been demonstrated by a close coincidence of the experimentally observed and calculated X-ray emission/absorption spectra, magnetic moments, density of states at the Fermi level, and electronic conductivity in the disordered non-stoichiometric SrFeO3-δ, SrFe0.75Mn0.25O3-δ, and SrFe0.85Co0.15O3-δ phases. The composition SrFe0.85Co0.15O3-δ is proposed as a promising electrode material with enhanced characteristics of electric transport.

Godbillon-Vey invariants of Non-Lorentzian spacetimes and Aristotelian hydrodynamics

We study the geometry of foliated non-Lorentzian spacetimes in terms of the Godbillon-Vey class of the foliation. We relate the intrinsic torsion of a foliated Aristotelian manifold to its Godbillon-Vey class, and interpret it as a measure of the local spin of the spatial leaves in the time direction. With this characterisation, the Godbillon-Vey class is an obstruction to integrability of the -structure defining the Aristotelian spacetime. We use these notions to formulate a new geometric approach to hydrodynamics of fluid flows by endowing them with Aristotelian structures. We establish conditions under which the Godbillon-Vey class represents an obstruction to steady flow of the fluid and prove new conservation laws.

A nitroxide-containing cathode material for organic radical batteries studied with pulsed EPR spectroscopy

An electron spin echo in a nitroxide-containing polymer cathode film for organic radical batteries is observed for various states of charge at cryogenic temperatures. The EPR-detected state of charge (ESOC), as inferred from the number of paramagnetic centers in the film, is compared to the results of Coulomb counting based on galvanostatic charging. Spin concentration, longitudinal relaxation times T1 and phase memory times Tm strongly correlate with the ESOC. In the discharged film, the spin concentration reaches 5±3×1020 cm−3, causing a phase memory time Tm≪ 100 ns (shorter than the resonator ring-down time) that hinders the detection of the spin echo. In the charged film, the decreased spin concentration results in a longer Tm between 100 ns and 300 ns that enables spin-echo detection, yet limits the length of the microwave pulse sequence. The short, broad-band pulses cause instantaneous diffusion in the unoxidized domains across the oxidized film, affecting the relative peak intensities in the pulsed EPR spectrum. By simulating the spectral distortion caused by instantaneous diffusion, we obtain information on the local spin concentration, which complements the information on the ‘bulk’ spin concentration determined by electrochemistry and continuous-wave EPR spectroscopy.

Spin current in the early stage of radical reactions and its mechanisms.

We study the electronic spin flux (atomic-scale flow of the spin density in molecules) by a perturbation analysis and abinitio nonadiabatic calculations. We derive a general perturbative expression of the charge and spin fluxes and identify the driving perturbation of the fluxes to be the time derivative of the electron-nucleus interaction term in the Hamiltonian. We then expand the expression in molecular orbitals so as to identify relevant components of the fluxes. Our perturbation theory describes the electronic fluxes in the early stage of reactions in an intuitively clear manner. The perturbation theory is then applied to an analysis of the spin flux obtained in abinitio calculations of the radical reaction of O2 and CH3· starting from three distinct spin configurations; (a) CH3· and triplet O2 with total spin of the system set Stot=1/2 (b) CH3· and singlet O2, Stot=1/2, and (c) CH3· and triplet O2, Stot=3/2. Further analysis of the time-dependent behaviors of the spin flux in these numerical simulations reveals (i) the spin flux induces rearrangement of the local spin structure, such as reduction of the spin polarization arising from the triplet O2 and (ii) the spin flux flows from O2 to CH3· in the reaction starting from spin configuration (a) and from CH3· to O2 in that starting from configuration (b), whereas no major intermolecular spin flux was observed in that starting from configuration (c). Our study thus establishes the mechanism of the spin flux that rearranges the local spin structures associated with chemical bonds.