Spin Polarization Research Articles

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.

Differences in Kondo Splitting of Surface Quantum Systems Induced by Two Distinct Magnetic Tips: A Joint Method of DFT and HEOM.

The interactions between a magnetic tip and local spin impurities initiate unconventional Kondo phenomena, such as asymmetric suppression or even splitting of the Kondo peak. However, a lack of realistic theoretical models and comprehensive explanations for this phenomenon persists due to the complexity of the interactions. This research employs a joint method of density functional theory (DFT) and hierarchical equation of motion (HEOM) to simulate and contrast the modulation of the spin state and Kondo behavior in the Fe/Cu(100) system with two distinct magnetic tips. A cobalt tip, possessing a larger magnetic moment, incites greater atomic displacement of the iron atom, more notable alterations in electronic structure, and enhanced charge transfer with the environment compared with the control process utilizing a nickel tip. Furthermore, the Kondo resonance undergoes asymmetric splitting as a result of the ferromagnetic correlation between the iron atom and the magnetic tip. The Co tip's higher spin polarization results in a wider spacing between the splitting peaks. This investigation underscores the precision of the DFT + HEOM approach in predicting complex quantum phenomena and explaining the underlying physical principles. This provides valuable theoretical support for developing more sophisticated quantum regulation experiments.

Enhanced Oxygen Evolution and Zinc-Air Battery Performance via Electronic Spin Modulation in Heterostructured Catalysts.

Beyond optimizing electronic energy levels, the modulation of the electronic spin configuration is an effective strategy, often overlooked, to boost activity and selectivity in a range of catalytic reactions, including the oxygen evolution reaction (OER). This electronic spin modulation is frequently accomplished using external magnetic fields, which makes it impractical for real applications. Herein, spin modulation is achieved by engineering Ni/MnFe2O4 heterojunctions, whose surface is reconstructed into NiOOH/MnFeOOH during the OER. NiOOH/MnFeOOH shows a high spin state of Ni, which regulates the OH- and O2 adsorption energy and enables spin alignment of oxygen intermediates. As a result, NiOOH/MnFeOOH electrocatalysts provide excellent OER performance with an overpotential of 261 mV at 10 mA cm-2. Besides, rechargeable zinc-air batteries based on Ni/MnFe2O4 show a high open circuit potential of 1.56 V and excellent stability for more than 1000 cycles. This outstanding performance is rationalized using density functional theory calculations, which show that the optimal spin state of both Ni active sites and oxygen intermediates facilitates spin-selected charge transport, optimizes the reaction kinetics, and decreases the energy barrier to the evolution of oxygen. This study provides valuable insight into spin polarization modulation by heterojunctions enabling the design of next-generation OER catalysts with boosted performance.

Field-free switching of perpendicular magnetization in a noncollinear antiferromagnetic Mn3Sn/[Pt/Co]4 heterostructure

Spin-orbit torque (SOT) manipulation of perpendicular magnetization is essential for realizing spintronic storage and logic devices. When a charge current flows through a heavy metal/ferromagnetic layer structure, a spin current can be generated by the heavy metal and injects into the ferromagnetic layer with perpendicular magnetic anisotropy and switch its magnetization via the SOT. However, in order to realize the deterministic switching, an in-plane external magnetic field is needed to break the inversion symmetry, a technological requirement that hampers the practical application of SOT. Pt/Co multilayer is a good magnetic recording media and, thus, the all-electric manipulation of its perpendicular magnetic moments is of practical significance. The noncollinear spin structure in Mn3Sn allows an unconventional spin polarization direction, and the associated SOT can switch the magnetic moments in the absence of an external field. In this work, we demonstrate the field-free SOT switching of a heterostructure utilizing Mn3Sn and Pt/Co multilayer as the spin source and the ferromagnetic layer with perpendicular magnetization, respectively. Our results are important for advancing the development of spintronic devices based on noncollinear antiferromagnets.

A dual spin-controlled chiral two-/three-dimensional perovskite artificial leaf for efficient overall photoelectrochemical water splitting

The oxygen evolution reaction, which involves high overpotential and slow charge-transport kinetics, plays a critical role in determining the efficiency of solar-driven water splitting. The chiral-induced spin selectivity phenomenon has been utilized to reduce by-product production and hinder charge recombination. To fully exploit the spin polarization effect, we herein propose a dual spin-controlled perovskite photoelectrode. The three-dimensional (3D) perovskite serves as a light absorber while the two-dimensional (2D) chiral perovskite functions as a spin polarizer to align the spin states of charge carriers. Compared to other investigated chiral organic cations, R-/S-naphthyl ethylamine enable strong spin-orbital coupling due to strengthened π–π stacking interactions. The resulting naphthyl ethylamine-based chiral 2D/3D perovskite photoelectrodes achieved a high spin polarizability of 75%. Moreover, spin relaxation was prevented by employing a chiral spin-selective L-NiFeOOH catalyst, which enables the secondary spin alignment to promote the generation of triplet oxygen. This dual spin-controlled 2D/3D perovskite photoanode achieves a 13.17% of applied-bias photon-to-current efficiency. Here, after connecting the perovskite photocathode with L-NiFeOOH/S-naphthyl ethylamine 2D/3D photoanode in series, the resulting co-planar water-splitting device exhibited a solar-to-hydrogen efficiency of 12.55%.

Probing the metallic state, magnetic anisotropy, and large Curie temperature in CaCuFeReO[formula omitted]: Strain engineering

Rhenium-based double perovskite oxides (DPOs) are a particularly fascinating class of materials because of high carrier spin polarization, large magnetic anisotropy energy (MAE), and complex electrical behavior along with high Curie temperature (TC). Herein, we discussed the impact of biaxial ([110]) strain ranging from −5% to ＋ 5% along the ab-plane on the electronic and magnetic properties of CaCuFeReO6 (CCFRO) DPO using ab-inito calculations. The unstrained system exhibits a ferrimagnetic (FiM) spin ordering as an energetically stable magnetic ground state due to electron hopping between Fe+3/Re+5t2g and Cu+2eg orbitals along with a metallic electronic state. Moreover, [010] (b-axis) is the magnetic easy axis that produces the MAE of 5.36 meV, giving a giant MAE constant of 1.97×107 erg/cm3. The evaluated partial spin-magnetic moment on the Cu1/Cu2/Fe/Re ion is 0.14/0.44/4.04/−0.64μB, where “−” sign on the Re moment means that its spin is antiparallel to the other ions, verifying the FiM ordering in the system. Also, the eg, t2g/eg, and t2g orbital characteristics of Cu+2, Fe+3, and Re+5 ions are visible in the spin-magnetization density iso-surfaces plots, respectively. Using the classical Heisenberg model, the computed TC for the unstrained structure is 576 K, which is quite close to the experimentally reported value of 567 K. In addition, it is shown that the FiM metallic behavior in the motif is robust against biaxial ([110]) strain within the considered range. It has also been revealed that TC increased to 5.73%/3.30% for the considered range of −5% compressive/＋5% tensile strain due to improved structural distortions.

Structural, magnetic and transport properties of FeRuVZ (Z = Si, Ge) Heusler alloys: Experiment and theory

Heusler alloys based on 4d-elements are relatively less explored though they are known to host interesting electronic/magnetic properties useful for future spintronics applications. Here, we report a comparative study of the structural and magnetic properties of FeRuVSi (FRVS) and FeRuVGe (FRVG) using experimental and theoretical tools. Magneto-transport measurements have also been carried out to probe the role of magnetism on their transport behaviour. Room temperature (T) X-ray diffraction data reveals cubic crystal structure (space group No. 216) with B2 type antisite disorder between Fe and Ru sites in both the alloys. They show ferromagnetic behaviour below the Curie temperature (TC) 84 K for FeRuVSi and 57 K for FeRuVGe respectively. The field dependence of magnetization at low-T shows saturating (nearly saturating) behaviour for FRVS (FRVG). Transport measurements show metallic behaviour with a sharp reduction in the resistivity near TC. Ab-initio calculations predict nearly half metallic behaviour with ∼ 87 % and ∼ 89 % spin polarization for FRVS and FRVG in their ordered states. The inclusion of antisite disorder changes the magnetic configuration, leading to a visible decrease in the magnetic moment and spin polarization. The calculated net moment and the transport properties agree fairly well with those observed experimentally. These results confirm the importance of disorder in determining the intrinsic properties of these alloys. Such combined studies help in the identification of more novel quantum materials suitable for future spintronic applications.

Boosting photoelectrochemical performance through appling magnetic field in manganese-doped cobalt ferrite photoanodes

An efficient photoelectrochemical water-splitting process is of paramount importance as it provides a sustainable and clean method for generating hydrogen fuel, which is crucial for addressing the world’s growing energy needs while mitigating environmental concerns. Herein, the effects of applying a magnetic field on the photoelectrochemical performance of photoanodes composed of Cobalt ferrite (CoFe2O4) and Manganese (Mn)-doped CoFe2O4 are investigated. The CoMnxFe2-xO4 nanoparticles were synthesized using a sol–gel method, with varying values of x (0.0, 0.1, 0.3, and 0.5). X-ray diffraction analysis consistently reveals a singular cubic spinel structure for all four samples. Magnetic analyses demonstrate an enhancement in magnetic characteristics, including saturation magnetization, coercivity, and anisotropy field in the CoMn0.3Fe1.7O4 sample compared to the other three samples. Photoelectrochemical (PEC) measurements indicate that the photocurrent increases in all four samples when a static magnetic field is applied. However, the CoMn0.3Fe1.7O4 sample shows a more pronounced enhancement. Specifically, the dark current density increases by more than 115 % when a magnetic field of 190 ± 20 mT is applied. Additionally, it rises by 387 % under light illumination with the magnetic field. This enhancement in PEC performance is attributed to electron spin polarization adjusted through the external magnetic field.

Multiple Pathways in the Triplet States Population for a Naphthalenediimide-C60 Dyad.

The link of an antenna dye with an electron spin converter, in this case naphthalenediimide and C60, produces a system with a rich photophysics including the detection of more than one triplet state on the long timescale (tens of µs). Beside the use of optical spectroscopies in the ns and in the fs time scale, we used time-resolved Electron Paramagnetic Resonance (TREPR) to study the system evolution following photoexcitation. TREPR keeps track of the formation path of the triplet states through specific spin polarization patterns observed in the spectra. The flexibility of the linker plays a role in favouring either electron transfer or energy transfer processes.

Half-metallic ferromagnetic and optical properties of YScO[formula omitted] (Y = Ni, Pd, and Pt) perovskite: A first principles study

In this paper, we investigate the electronic, magnetic, and optical properties of scandium based ternary oxides perovskite YScO3 (Y = Ni, Pd, Pt). We employ the Tran and Blaha modified Becke-Johnson approximation to calculate spin polarization using the density functional theory. Based on the formation energy, we found that our materials are thermodynamically stable (−0.76 eV, −1.3 eV and −1.65 eV for NiScO3, PdScO3 and PtScO3, respectively). The densities of states and spin polarized band structures for spin up (↑) and spin down (↓) channels reveal the half-metallic nature for all studied compounds with Ni/Pd/Pt-d orbitals playing a major role in the valence band. Additionally, all perovskites exhibit ferromagnetic behavior with magnetic moments approximately equal to 3 μB. Moreover, we calculate several optical parameters such as the dielectric constants, refractive index, reflectivity, extinction and absorption coefficients for these compounds. The results suggest that these perovskites might be promising candidates for optical and spintronic devices.

Voltage tunable sign inversion of magnetoresistance in van der Waals Fe3GeTe2/MoSe2/Fe3GeTe2 tunnel junctions

The magnetic tunnel junctions (MTJs) based on van der Waals (vdW) materials possess atomically smooth interfaces with minimal element intermixing. This characteristic ensures that spin polarization is well maintained during transport, leading to the emergence of richer magnetoresistance behaviors. Here, using all 2D vdW MTJs based on magnetic metal Fe3GeTe2 and non-magnetic semiconductor MoSe2, we demonstrate that the magnitude and even sign of the magnetoresistance can be tuned by the applied voltage. The sign inversion of the magnetoresistance is observed in a wide temperature range below the Curie temperature. This tunable magnetoresistance sign may be attributed to the spin polarizations of the tunneling carriers and the band structure of the two ferromagnetic electrodes. Such robust electrical tunability of magnetoresistance extends the functionalities of low-dimensional spintronics and makes it more appealing for next-generation spintronics with all-vdW MTJs.

Alternant Hydrocarbon Diradicals as Optically Addressable Molecular Qubits.

High-spin molecules allow for bottom-up qubit design and are promising platforms for magnetic sensing and quantum information science. Optical addressability of molecular electron spins has also been proposed in first-row transition-metal complexes via optically detected magnetic resonance (ODMR) mechanisms analogous to the diamond-nitrogen-vacancy color center. However, significantly less progress has been made on the front of metal-free molecules, which can deliver lower costs and milder environmental impacts. At present, most luminescent open-shell organic molecules are π-diradicals, but such systems often suffer from poor ground-state open-shell characters necessary to realize a stable ground-state molecular qubit. In this work, we use alternancy symmetry to selectively minimize radical-radical interactions in the ground state, generating π-systems with high diradical characters. We call them m-dimers, referencing the need to covalently link two benzylic radicals at their meta carbon atoms for the desired symmetry. Through a detailed electronic structure analysis, we find that the excited states of alternant hydrocarbon m-diradicals contain important symmetries that can be used to construct ODMR mechanisms leading to ground-state spin polarization. The molecular parameters are set in the context of a tris(2,4,6-trichlorophenyl)methyl (TTM) radical dimer covalently tethered at the meta position, demonstrating the feasibility of alternant m-diradicals as molecular color centers.

Electrostatically controlled spin polarization in Graphene-CrSBr magnetic proximity heterostructures

The magnetic proximity effect can induce a spin dependent exchange shift in the band structure of graphene. This produces a magnetization and a spin polarization of the electron/hole carriers in this material, paving the way for its use as an active component in spintronics devices. The electrostatic control of this spin polarization in graphene has however never been demonstrated so far. We show that interfacing graphene with the van der Waals antiferromagnet CrSBr results in an unconventional manifestation of the quantum Hall effect, which can be attributed to the presence of counterflowing spin-polarized edge channels originating from the spin-dependent exchange shift in graphene. We extract an exchange shift ranging from 27 – 32 meV, and show that it also produces an electrostatically tunable spin polarization of the electron/hole carriers in graphene ranging from − 50% to + 69% in the absence of a magnetic field. This proof of principle provides a starting point for the use of graphene as an electrostatically tunable source of spin current and could allow this system to generate a large magnetoresistance in gate tunable spin valve devices.

Effects of tensor spin polarization on the chiral restoration and deconfinement phase transitions

Effects of tensor spin polarization (TSP) on the chiral restoration and deconfinement phase transitions are studied in Polyakov loop extended Nambu–Jona-Lasinio (PNJL) model. For chiral phase transition, the higher the polarized degree of quark-antiquark pairs under the strong magnetic field, the higher the phase transition temperature. The TSP corrects the position of the critical end point. The small impact of TSP on the phase transition temperature is found for the deconfinement phase transition. On the other hand, we divide the phase space into three ranges based on the phase diagram obtained from the PNJL model: the confinement phase with chiral symmetry broken, the deconfinement phase with restored chiral symmetry, and the confinement phase with restored chiral symmetry (quarkyonic phase). It is found that TSP has only a very small effect on the anisotropic pressure in the deconfined phase with chiral symmetry restored and the quarkyonic phase, but it has a very strong effect on the anisotropic pressure in the confined phase with chiral symmetry broken. This is because TSP is closely related to chiral symmetry. The restoration of chiral symmetry means the dissociation of spin polarization condensate. Published by the American Physical Society 2024

Strain-induced giant enhancement and transformation of magnetocrystalline anisotropy in 1T-FeSe2 monolayer

The development of magnetic materials with large magnetic anisotropy energy (MAE) is crucial for magnetic storage and spintronics applications. The electronic structure and magnetic properties of 1T-FeSe2 monolayer have been systematically investigated by first-principles computational methods. The monolayer 1T-FeSe2 is confirmed to be a ferromagnetic semimetal with 100% spin polarization and exhibits pronounced magnetic anisotropy. It shows an easy magnetization plane in the two-dimensional plane and its MAE is as high as 8.134 meV. The MAE mainly originates from the contributions of transitions between Fe dyz and dz2, dxy and dx2−y2 orbitals, while the contributions of transitions between p x and p y, p x and p z orbitals of Se are also obvious. The biaxial strain significantly regulates the magnetic properties and electronic structures of the 1T-FeSe2 monolayer. Interestingly, the MAE increases significantly to 77.680 meV when the tensile strain increases to 3.5%, we can expect to achieve a reasonable value of MAE up to 98.951 meV by applying 5% tensile strain. In addition, the easy magnetization plane changes to perpendicular easy magnetization axis direction at −6% compressive strain or 7% tensile strain, which leads to a significant change in the band structure near the Fermi level. The 100% spin-polarized ferromagnetic semi-metallic behavior and the huge strain-induced magnetic anisotropy make the 1T-FeSe2 monolayer material promising for spintronics and magnetic data storage.

Probing the electronic structure, optical, and transport nature of lanthanide-based ternary materials: A First-principles perspective

High thermal stability and adjustable optoelectronic properties are the unique characteristics of lanthanide-based materials. The complex interplay between unique electronic, optical, and thermoelectric characteristics of lanthanide-based ternary chalcogenides is investigated by first principles modeling. The cohesive energy values were anticipated to be −4.54 eV/atom for PrSF and −4.87 eV/atom for PrSBr suggesting PrSBr to have the greatest bonding properties and is the most stable material. The computed formation energies range from −1.3 to −3.0 (eV/f. u), demonstrating their stability. The inclusion of bromine, a more electronegative element than fluorine, produces unique hybridization patterns and spin polarization effects. Compared to PrSBr, PrSF bonding employs more effective orbital hybridization, resulting in a greater band gap. PrSF has a higher frequency dielectric constant compared to PrSBr. The absorption edges in the ε2(ω) result from optical transitions between the Pr-f, S-p, F-p, and Br-p states. As the temperature rises, the Seeback coefficients for PrSF and PrSBr decrease exponentially. The thermal conductivity spectra of PrSF and PrSBr materials exhibit a linear increase across the temperature range. As temperature rises, the concentration of carriers and mobility increases, resulting in increased electrical conductivity values.

Structural and Electronic Chirality in Inorganic Crystals: from Construction to Application.

Chirality represents a fundamental characteristic inherent in nature, playing a pivotal role in the emergence of homochirality and the origin of life. While the principles of chirality in organic chemistry are well-documented, the exploration of chirality within inorganic crystal structures continues to evolve. This ongoing development is primarily due to the diverse nature of crystal/amorphous structures in inorganic materials, along with the intricate symmetrical and asymmetrical relationships in the geometry of their constituent atoms. In this review, we commence with a summary of the foundational concept of chirality in molecules and solid states matters. This is followed by an introduction of structural chirality and electronic chirality in three-dimensional and two-dimensional inorganic materials. The construction of chirality in inorganic materials is classified into physical photolithography, wet-chemistry method, self-assembly, and chiral imprinting. Highlighting the significance of this field, we also summarize the research progress of chiral inorganic materials for applications in optical activity, enantiomeric recognition and chiral sensing, selective adsorption and enantioselective separation, asymmetric synthesis and catalysis, and chirality-induced spin polarization. This review aims to provide a reference for ongoing research in chiral inorganic materials and potentially stimulate innovative strategies and novel applications in the realm of chirality.

Negative spin polarization of Mn2VGa Heusler alloy thin films studied in current-perpendicular-to-plane giant magnetoresistance devices

Negative spin polarization of Mn2VGa Heusler alloy thin films studied in current-perpendicular-to-plane giant magnetoresistance devices

Pd(II) coordination molecule modified g-C3N4 for boosting photocatalytic hydrogen production

The photocatalytic H2 production activity of polymer carbon nitride (g-C3N4) is limited by the rapid recombination of photoelectron-hole pairs and slow surface reduction dynamic process. Here, a supramolecular complex (named R-TAP-Pd(II)) was fabricated via self-assembly of (R)-N-(1-phenylethyl)-4-(4-(pyridin-2-yl)-1H-1,2,3-triazol-1-yl)benzamide (R-TAP) with Pd(II) and used to modify g-C3N4. In the R-TAP-Pd(II)@g-C3N4 composite photocatalyst, the spin polarization of R-TAP-Pd(II) can promote charge transfer and inhibit photogenerated carrier recombination, as confirmed by spectral tests and photoelectrochemical performance tests. Electrochemical tests and in situ X-ray photoelectron spectroscopy (XPS) tests proved that the Pd(II) ion in the R-TAP-Pd(II) molecule can serve as active sites to accelerate H2 production. The R-TAP-Pd(II)@g-C3N4 presented a photocatalytic H2 generation rate of 1085 μmol g−1 h−1 when exposed to visible light, which was a about 278-fold increase compared with g-C3N4. This work finds a new approach to boost the photocatalytic efficiency of g-C3N4 via supramolecular self-assembly.

Uncovering the spin ordering in magic-angle graphene via edge state equilibration

The flat bands in magic-angle twisted bilayer graphene (MATBG) provide an especially rich arena to investigate interaction-driven ground states. While progress has been made in identifying the correlated insulators and their excitations at commensurate moiré filling factors, the spin-valley polarizations of the topological states that emerge at high magnetic field remain unknown. Here we introduce a technique based on twist-decoupled van der Waals layers that enables measurement of their electronic band structure and–by studying the backscattering between counter-propagating edge states–the determination of the relative spin polarization of their edge modes. We find that the symmetry-broken quantum Hall states that extend from the charge neutrality point in MATBG are spin unpolarized at even integer filling factors. The measurements also indicate that the correlated Chern insulator emerging from half filling of the flat valence band is spin unpolarized and suggest that its conduction band counterpart may be spin polarized.