Spin-polarized States Research Articles

Visualization of spin-polarized surface resonances in Pb-based ternary topological insulators

The formation of the topological surface state originates from bulk band inversion at the top of the valence band and the bottom of the conduction band. The transition between normal and topological insulators is known as a topological phase transition. Here we show spin-polarized electronic states of Pb-based ternary topological insulators Pb(Bi1-xSbx)2Te4 (x = 0.55, 0.70, 0.79) investigated by spin- and angle-resolved photoemission spectroscopy and first-principles calculations. We visualize a pair of spin-polarized surface resonances dispersing along the upper edge of projected bulk bands in occupied states. Interestingly, a branch of the spin-polarized surface resonances continuously connects to the topological surface state. The coexistence of the topological surface state and the spin-polarized surface resonances can be explained by considering the topological phase transition.

Magnetic Order in Nanogranular Iron Germanium (Fe0.53Ge0.47) Films.

We study the effect of strain on the magnetic properties and magnetization configurations in nanogranular FexGe1-x films (x = 0.53 ±0.05) with and without B20 FeGe nanocrystals surrounded by an amorphous structure. Relaxed films on amorphous silicon nitride membranes reveal a disordered skyrmion phase while films near and on top of a rigid substrate favor ferromagnetism and an anisotropic hybridization of Fe d levels and spin-polarized Ge sp band states. The weakly coupled topological states emerge at room temperature and become more abundant at cryogenic temperatures without showing indications of pinning at defects or confinement to individual grains. These results demonstrate the possibility to control magnetic exchange and topological magnetism by strain and inform magnetoelasticity-mediated voltage control of topological phases in amorphous quantum materials.

Spin polarization and transport of hybrid interface states in π-stacked magnetic molecular junctions

Based on the first-principles method, the spin polarization and transport properties of the hybrid interface states (HIS) in π-stacked three-layer triphenylene molecular junction are studied theoretically. By rotating the torsion angle between two neighbor layers, the π-π interaction strength is adjusted. The results demonstrate that the HIS, generated by strong pz-d hybridization between molecules and ferromagnetic electrodes, can easily transfer to the central layer via a strong π-π interaction with similar spin polarization. A weak π-π interaction will block the transfer of the HIS, where the discrete molecular orbital states dominate the central molecule. However, an enhancement of the spin polarization for the molecular frontier orbital states is observed. The transport calculation shows that efficient transport of the HIS is realized in the π-stacked system, where the largest current appears at a strong π-π interaction but a significant current spin polarization appears at a weak π-π interaction. This work deepens our understanding of the role of the HIS in π-stacked organic systems.

Robust topological insulating property in C2X-functionalized III-V monolayers

Two-dimensional topological insulators (TIs) show great potential applications in low-power quantum computing and spintronics due to the spin-polarized gapless edge states. However, the small bandgap limits their room-temperature applications. Based on first-principles calculations, a series of C2X (X = H, F, Cl, Br and I) functionalized III-V monolayers are investigated. The nontrivial bandgaps of GaBi-(C2X)2, InBi-(C2X)2, TlBi-(C2X)2and TlSb-(C2X)2are found to between 0.223 and 0.807 eV. For GaBi-(C2X)2and InBi-(C2X)2, the topological insulating properties originate from thes-px,yband inversion induced by the spin-orbital coupling (SOC) effect. While for TlBi-(C2X)2and TlSb-(C2X)2, the topological insulating properties are attributed to the SOC effect-induced band splitting. The robust topological characteristics are further confirmed by topological invariantsZ2and the test under biaxial strain. Finally, two ideal substrates are predicted to promote the applications of these TIs. These findings indicate that GaBi-(C2X)2, InBi-(C2X)2, TlBi-(C2X)2and TlSb-(C2X)2monolayers are good candidates for the fabrication of spintronic devices.

Manipulating Charge-to-Spin conversion via insertion layer control at the interface of topological insulator and ferromagnet

Strong spin–orbit coupling and highly spin-polarized surface states in topological insulators (TIs) are key parameters that explain their extremely high charge-to-spin conversion (CSC) efficiency at interfaces with ferromagnetic materials (FMs). This study focused on the influence of the insertion layer on the proximity effect occurring in a Co4Fe4B2/Bi2Se3 interface. Various insertion layers, including Au, MgO, and Se, were introduced to modulate the proximity effect from TI to FM and vice versa. X-ray photoelectron spectroscopy and transmission electron microscopy revealed that the Se insertion layer effectively suppresses the formation of an additional Bi layer, reducing intermixing against Co4Fe4B2. Electrical transport properties such as RXX and RXY under a vertical magnetic field show that the Se-inserted structure features the lowest anomalous Hall angle and exhibits a pristine topological surface state, indicating its potential for improving CSC efficiency. The Se-inserted structure exhibits the highest spin Hall angle among various heterostructures, according to results obtained from spin-torque ferromagnetic resonance. These findings highlight the importance of selecting an insertion layer and controlling the interface to optimize the spin-transport properties of TI-based spintronic devices and provide insights into the design of future spin devices.

Unconventional Discontinuous Transitions in Isospin Systems.

We show that two-dimensional fermions with dispersion k^{2} or k^{4} undergo a first-order Stoner transition to a fully spin-polarized state despite the fact that the spin susceptibility diverges at the critical point. We extend our analysis to systems with dispersion k^{2α} and spin and valley isospin and show that there is a cascade of instabilities into fractional-metal states with some electron bands fully depleted; narrow intermediate ranges of partially depleted bands exist for α<1 or α>2. The susceptibility becomes large near each transition. We discuss applications to biased bi- and trilayer graphene and moiré systems.

Few-shot learning for screening 2D Ga2CoS4−x supported single-atom catalysts for hydrogen production

Hydrogen generation and related energy applications heavily rely on the hydrogen evolution reaction (HER), which faces challenges of slow kinetics and high overpotential. Efficient electrocatalysts, particularly single-atom catalysts (SACs) on two-dimensional (2D) materials, are essential. This study presents a few-shot machine learning (ML) assisted high-throughput screening of 2D septuple-atomic-layer Ga2CoS4−x supported SACs to predict HER catalytic activity. Initially, density functional theory (DFT) calculations showed that 2D Ga2CoS4 is inactive for HER. However, defective Ga2CoS4−x (x = 0–0.25) monolayers exhibit excellent HER activity due to surface sulfur vacancies (SVs), with predicted overpotentials (0–60 mV) comparable to or lower than commercial Pt/C, which typically exhibits an overpotential of around 50 mV in the acidic electrolyte, when the concentration of surface SV is lower than 8.3%. SVs generate spin-polarized states near the Fermi level, making them effective HER sites. We demonstrate ML-accelerated HER overpotential predictions for all transition metal SACs on 2D Ga2CoS4−x. Using DFT data from 18 SACs, an ML model with high prediction accuracy and reduced computation time was developed. An intrinsic descriptor linking SAC atomic properties to HER overpotential was identified. This study thus provides a framework for screening SACs on 2D materials, enhancing catalyst design.

Doping the Spin-Polarized Graphene Minicone on Ni(111).

In the attempt to induce spin-polarized states in graphene (Gr), rare-earth deposition on Gr/Co(0001) has been demonstrated to be a successful strategy: the coupling of graphene with the cobalt substrate provides spin-polarized conical-shaped states (minicone) and the rare-earth deposition brings these states at the Fermi level. In this manuscript, we theoretically explore the feasibility of an analogue approach applied on Gr/Ni(111) doped with rare-earth ions by means of density functional theory calculations. Even if not well mentioned in the literature, this system owns a minicone, similar to the cobalt case. By testing different rare-earth ions, not only do we suggest which one can provide the required doping but we also explain the effect behind this proper charge transfer.

Investigation into the impact of anionic substitution on modulating the optical and catalytic properties of bismuth ferrite nanoparticles

Bismuth ferrite (BFO) nanoparticles have emerged as a non-toxic catalyst with remarkable potential for the photodegradation of various environmental pollutants. A notable departure from conventional approaches, where cations are added as dopant, this study achieved enhanced catalytic performance through anion substitution. Specifically, replacing oxygen atoms with nitrogen introduces spin-polarized defect states within the BFO’s energy gap, resulting in a notable reduction in the energy band gap. Nitrogen doping of bismuth ferrite yields a novel material with exceptional capabilities for the photodegradation of methylene blue dye and the reduction of 4-nitrophenol. Comprehensive characterization, including X-ray diffraction, Fourier-transform infrared spectroscopy, energy-dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy, has unequivocally confirmed the successful incorporation of nitrogen into the BFO nanoparticle lattice. Interestingly, field emission scanning electron microscopy analysis revealed no significant alteration in nanoparticle size after nitrogen doping. Meanwhile, UV-diffuse reflectance spectroscopy unveiled a distinct decrease in the energy gap upon nitrogen incorporation. The observed improvements in catalytic activities can be attributed to nitrogen ions, introduced as substitutes, effectively occupying the oxygen defects within the sample, thereby diminishing recombination centers for photogenerated charge carriers and decreasing recombination rates. Additionally, adsorption kinetics studies underscore the efficacy of the catalyst surface in adsorbing methylene blue and/or 4-nitrophenol, conforming to the Ho pseudo-second-order model. This study not only highlights the exciting potential of nitrogen-doped bismuth ferrite nanoparticles in environmental remediation but also sheds light on the intricate interplay between anion substitution, band structure modification, and catalytic performance enhancement.Graphical

Impact of Fe-doping on magneto-optoelectronic properties of beryllium sulfide (BeS): A first principles insight

The investigation of electronic, magnetic, structural, and optical properties of Be1-xFexS alloys is carried out by utilizing FP-LAPW method based on density functional theory (DFT) calculations. Fe-doped BeS exhibits half-metallic ferromagnetic behaviour at all doping concentrations, transforming it as favourable contender for spintronic devices. Our findings reveal the presence of 100 % spin polarization of electronic states. The calculated values of magnetic moments are 4.0, 8.0, and 16.0 μB for Be0.9375Fe0.0625S, Be0.875Fe0.125S and Be0.75Fe0.25S, respectively. The pristine BeS compound adopts a cubic close packing structure, known as the zinc blende structure, with the space group F-43m. The static values of R(0) are observed to be 0.21, 0.56, and 0.72 for Fe doped BeS at Be0.9375Fe0.0625S, Be00875Fe0.125S and Be0.75Fe0.25S, respectively. The maximum values of σ(ω) are computed as 16375.9 (1/Ω cm) for 6.25 %, 14336.5 (1/Ω cm) for 12.5 %, and 11002.1 (1/Ω cm) for 25 % Fe doped BeS. The present study unveils maximum optical absorption and conductivity in the ultraviolet (UV) region, suggesting its potential application in UV-based photovoltaic devices.

Towards robust dichroism in angle-resolved photoemission

Dichroic techniques are highly relevant in the field of topological materials, layered systems, and spin-polarized electronic states. Dichroism in angle-resolved photoemission is per se a matrix element effect, which depends on the initial and final states as well as on the perturbation by the light field. Although matrix element effects in ARPES such as dichroism are important for addressing properties of the initial state wave functions, the results can strongly depend on experimental geometry or final state effects. Combining experimental data on bulk WSe2 taken at soft x-ray photon energies with state-of-the-art photoemission calculations, we demonstrate that a dichroic observable called time-reversal dichroism remains unaffected against variation of photon energy, light polarization, and the angle of incidence. We demonstrate a direct link of TRDAD obtained with both linearly and circularly polarized photons to the initial state properties indicating its broad applicability. The robustness of this matrix element effect indicates a considerable benefit over other dichroic techniques and encourages further experimental and theoretical investigations.

Anomalous Landau Level Gaps Near Magnetic Transitions in Monolayer WSe2

First-order phase transitions produce abrupt changes to the character of both ground and excited electronic states. Here we conduct electronic compressibility measurements to map the spin phase diagram and Landau level (LL) energies of monolayer WSe2 in a magnetic field. We resolve a sequence of first-order phase transitions between completely spin-polarized LLs and states with LLs of both spins. Unexpectedly, the LL gaps are roughly constant over a wide range of magnetic fields below the transitions, which we show reflects spin-polarized ground states with opposite spin excitations. These transitions also extend into compressible regimes, with a sawtooth boundary between full and partial spin polarization. We link these observations to the important influence of LL filling on the exchange energy beyond a smooth density-dependent contribution. Our results show that WSe2 realizes a unique hierarchy of energy scales where such effects induce reentrant magnetic phase transitions tuned by density and magnetic field. Published by the American Physical Society 2024

First-principles studies of the stability, structural, electronic, magnetic and optical properties of halogen atom doped marcasite FeS2

The effects of halogen atom (F, Cl, Br or I) doping on the stability, structural, electronic, magnetic and optical properties of marcasite FeS2 (m-FeS2) are investigated through the first-principles calculations. The formation energies are relatively small under Fe-rich condition, indicating that it is feasible to implant halogen atom into m-FeS2. The ground state of halogen atom doped m-FeS2 systems is magnetic due to the positive energy differences between non-spin-polarized and spin-polarized states. Phonon dispersion curves show that all doping systems are dynamically stable. The total magnetic moment of all doping systems is nearly 1μB, since replacing the S atom with a halogen atom introduces a non-bonding electron. Most of them come from Fe and S atoms, and only a small fraction come from the dopant. The simulation results show that F- and Br-doped m-FeS2 systems are still semiconductors although the band gaps are reduced considerably, Cl-doped m-FeS2 changes to a half-metal with half metallic band gap of 0.25 eV, while I-doped m-FeS2 becomes a metal, making them potentially useful in spintronics. In addition, the halogen atom doped m-FeS2 systems possess enhanced absorption coefficient and red-shifted absorption edge. So they are promising in optoelectronic device and solar energy harvesting.

Spin-polarized DFT investigations of novel KVSb half-Heusler compound for spintronic and thermodynamic applications

In this study we have investigated the robust phase stability, elasto-mechanical, thermophysical and magnetic response of KVSb half Heusler compound by implementing density functional theory (DFT) models in WIEN2k simulation package. The dynamic phase stability is computed in phase type I, II & III phase configurations by optimising their energy. It is observed that given compound is more stable in spin-polarized state of phase type-III. To explore the electronic band structure, we apply the generalised gradient approximation along with Hubbard potential U. The electronic band profile of the Heusler alloy display a half-metallic nature. Moreover, the calculated second-order elastic parameters divulge the brittle nature. To understand the thermodynamical and thermoelectric stability of the alloy at various temperature and pressures ranges Quasi-Harmonic Debye model is executed successfully. The computed value of magnetic moment (MM) found in good agreement with Slater-Pauling rule. Our findings confirms that the predicted half Heusler alloy can be used in various spintronics and thermoelectric applications.

Nematic Metal in a Multivalley Electron Gas: Variational MonteCarlo Analysis and Application to AlAs.

The two-dimensional electron gas is of fundamental importance in quantum many-body physics. We study a minimal extension of this model with C_{4} (as opposed to full rotational) symmetry and an electronic dispersion with two valleys with anisotropic effective masses. Electrons in our model interact via Coulomb repulsion, screened by distant metallic gates. Using variational MonteCarlo simulations, we find a broad intermediate range of densities with a metallic valley-polarized, spin-unpolarized ground state. Our results are of direct relevance to the recently discovered "nematic" state in AlAs quantum wells. For the effective mass anisotropy relevant to this system, m_{x}/m_{y}≈5.2, we obtain a transition from an anisotropic metal to a valley-polarized metal at r_{s}≈12 (where r_{s} is the dimensionless Wigner-Seitz radius). At still lower densities, we find a (possibly metastable) valley and spin-polarized state with a reduced electronic anisotropy.

Electrostatic doping tunable magnetic transition and half-metallicity in the monolayer CrCTe3

The electrical manipulation of the magnetic transition and spin-polarized states has attracted extensive attention in the field of spintronics. In this work, we perform a detailed study on the electronic and magnetic properties of the carrier-doped monolayer CrCTe3 by using first-principles calculation. It is found that, the magnetic transition from Néel-antiferomagnetic (nAFM) to ferromagnetic (FM) is observed in the case of the electron doping, while for hole doping a magnetic transition sequence of nAFM → zigzag-AFM → FM is observed in the monolayer CrCTe3. Interestingly, the carrier doping induced FM ground state always exhibits half-metallicity with full spin polarization. Moreover, the spin polarity of the half-metallic electronic states is opposite for electron and hole doping, meaning that the spin polarization direction can be tuned by manipulating a gate voltage. The Monte Carlo calculations show that the magnetic transition temperature of the doped FM CrCTe3 is rapidly increased with the increasing doping concentration and is extremely expected to achieve room temperature at a suitable doping concentration. These findings demonstrate that the monolayer AFM system possesses a potential application in spintronic devices with electrically tunable spin polarization.

Observation of edge states derived from topological helix chains.

Introducing the concept of topology has revolutionized materials classification, leading to the discovery of topological insulators and Dirac-Weyl semimetals1-3. One of the most fundamental theories underpinning topological materials is the Su-Schrieffer-Heeger (SSH) model4,5, which was developed in 1979-decades before the recognition of topological insulators-to describe conducting polymers. Distinct from the vast majority of known topological insulators with two and three dimensions1-3, the SSH model predicts a one-dimensional analogue of topological insulators, which hosts topological bound states at the endpoints of a chain4-8. To establish this unique and pivotal state, it is crucial to identify the low-energy excitations stemming from bound states, but this has remained unknown in solids because of the absence of suitable platforms. Here we report unusual electronic states that support the emergent bound states in elemental tellurium, the single helix of which was recently proposed to realize an extended version of the SSH chain9,10. Using spin- and angle-resolved photoemission spectroscopy with a micro-focused beam, we have shown spin-polarized in-gap states confined to the edges of the (0001) surface. Our densityfunctional theory calculations indicate that these states are attributed to the interacting bound states originating from the one-dimensional array of SSH tellurium chains. Helices in solids offer a promising experimental platform for investigating exotic properties associated with the SSH chain and exploring topological phases through dimensionality control.

Large-Substrate-Terrace Confined Growth of Arrayed Ultrathin PtSe2 Ribbons on Step-Bunched Vicinal Au(001) Facets Toward Electrocatalytic Applications.

Ultrathin PtSe2 ribbons can host spin-polarized edge states and distinct edge electrocatalytic activity, emerging as a promising candidate for versatile applications in various fields. However, the direct synthesis is still challenging and the growth mechanism is still unclear. Herein, the arrayed growth of ultrathin PtSe2 ribbons on bunched vicinal Au(001) facets, via a facile chemical vapor deposition (CVD) route is reported. The ultrathin PtSe2 flakes can transform from traditional irregular shapes to desired ribbon shapes by increasing the height of bunched and unidirectionally oriented Au steps (with step height hstep) is found. This crossover, occurring at hstep ≈ 3.0nm, defines the tailored growth from step-flow to single-terrace-confined modes, as validated by density functional theory calculations of the different system energies. On the millimeter-scale single-crystal Au(001) films with aligned steps, the arrayed ultrathin PtSe2 ribbons with tunable width of ≈20-1000nm, which are then served as prototype electrocatalysts for hydrogen evolution reaction (HER) is achieved. This work should represent a huge leap in the direct synthesis and the mechanism exploration of arrayed ultrathin transition-metal dichalcogenides (TMDCs) ribbons, which should stimulate further explorations of the edge-related physical properties and practical applications.

Electronic and magnetic properties of Me-Graphene nanoribbons: A DFT investigation

In the search for semiconducting materials at the nanoscale, theoretical methods have been used to propose a series of nanocarbon sheets featuring a mixture of sp2 and sp3 hybridized carbon atoms, with Me-Graphene as one example. In addition to interesting physical properties shown by these 2D forms, nanoribbon variations of these structures can feature new properties. In this work, we show that the electronic properties of Me-Graphene nanoribbons can be modulated through structural details such as chirality, width, and edge details. Not only the metallic or semiconducting behavior can be switched by choosing selected geometries, but the direct or indirect character of the gap of the semiconducting cases can be triggered by selecting specific chiralities. In particular combinations of chirality and edge structure, we further point out that multiple spin-polarized states emerge, turning these systems into potential materials for spintronics.

High-temperature concomitant metal-insulator and spin-reorientation transitions in a compressed nodal-line ferrimagnet Mn3Si2Te6

Symmetry-protected band degeneracy, coupled with a magnetic order, is the key to realizing novel magnetoelectric phenomena in topological magnets. While the spin-polarized nodal states have been identified to introduce extremely-sensitive electronic responses to the magnetic states, their possible role in determining magnetic ground states has remained elusive. Here, taking external pressure as a control knob, we show that a metal-insulator transition, a spin-reorientation transition, and a structural modification occur concomitantly when the nodal-line state crosses the Fermi level in a ferrimagnetic semiconductor Mn3Si2Te6. These unique pressure-driven magnetic and electronic transitions, associated with the dome-shaped Tc variation up to nearly room temperature, originate from the interplay between the spin-orbit coupling of the nodal-line state and magnetic frustration of localized spins. Our findings highlight that the nodal-line states, isolated from other trivial states, can facilitate strongly tunable magnetic properties in topological magnets.