Spin Polarization Research Articles

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.

Deep polarization of the ensemble nitrogen-vacancy centers in diamonds induced by an Airy beam with a long focal depth

Solid-state spin systems with nitrogen-vacancy (NV) centers in diamonds constitute an increasingly popular platform for quantum sensing. However, most existing platforms designed with ensemble NV centers exhibit a sensitivity that is significantly less than the theoretical maximum. This low sensitivity limits the expansion of the experimental results and application areas. In this study, the sensitivity is improved by increasing the pumping depth of the excitation beam to increase the number of particles involved in spin polarization at a given laser intensity. Compared with the proposed Airy beam with a long focal depth (25.46 λ) and the widely utilized Gauss beam pumping ensemble NV centers, the spin resonance factor fSR can be improved by 10.02%. This sensitivity-optimized approach enhances the functionality of sensors with NV centers.

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.

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.

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

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.

Triplet Excited State Mechanistic Study of meso‐Substituted Methylthio Bodipy Derivative: Time‐Resolved Optical and Electron Paramagnetic Resonance Spectral Studies

AbstractUnderstanding the intersystem crossing (ISC) mechanism of organic compounds is essential for designing new triplet photosensitizers. Herein, we investigated the ISC mechanism of a heavy atom‐free Bodipy derivative with thiomethyl substitution (S−BDP). A long‐lived triplet state was observed with nanosecond transient absorption spectroscopy with lifetime of 7.5 ms in a polymer film and 178 μs intrinsic lifetime in fluid solution, much longer as compared with what was previously reported (apparent triplet lifetime=15.5 μs). Femtosecond transient absorption studies retrieved an ISC time constant of ∼3 ns. Time‐resolved electron paramagnetic resonance (TREPR) indicated a special triplet electron spin polarization phase (ESP) pattern (a, e, a, e, a, e) for S−BDP, different from the ESP (e, e, e, a, a, a) typical for the spin‐orbital coupling (SOC) mechanism. This indicates that the electron spin selectivity of the ISC of S−BDP is different from that of the normal SOC effect in iodo‐Bodipy. Simulations of the TREPR spectra give a zero‐field‐splitting D parameter of −2257 MHz, much smaller as compared to the reference 2,6‐diiodo‐Bodipy (D=−4380 MHz). The computed SOC matrix elements (0.28–1.59 cm−1) and energy gaps for the S1/Tn states suggest that the energy matching between the S1 and T2/T3 states (supported by the largest kISC ∼109 s−1) enhances the ISC for this compound.

Attraction from kinetic frustration in ladder systems

We analyze the formation of multiparticle bound states in ladders with frustrated kinetic energy in two-component bosonic and two-component fermionic systems. We focus on the regime of light doping relative to insulating states at half-filling, spin polarization close to 100%, and strong repulsive interactions. A special feature of these systems is that the binding energy scales with single-particle tunneling t rather than exchange interactions, since effective attraction arises from alleviating kinetic frustration. For two-component Fermi systems on a zigzag ladder we find a bound state between a hole and a flipped spin (magnon) with a binding energy that can be as large as 0.6t. We demonstrate that magnon-hole attraction leads to formation of clusters comprising several holes and magnons, and we expound on antiferromagentic correlations for the transverse spin components inside the clusters. We identify several many-body states that result from self-organization of multiparticle bound states, including a Luttinger liquid of hole-magnon pairs and a density wave state of two-hole–three-magnon composites. We establish a symmetry between the spectra of Bose and Fermi systems and use it to establish the existence of antibound states in two-component Bose mixtures with SU(2) symmetric repulsion on a zigzag ladder. We also consider Bose and Fermi systems on a square ladder with flux and demonstrate that both systems support bound states. We discuss experimental signatures of multiparticle bound states in both equilibrium and dynamical experiments. We point out intriguing connections between these systems and the quark bag model in QCD. Published by the American Physical Society 2024

Engineering Spatially Adjacent Redox Sites with Synergistic Spin Polarization Effect to Boost Photocatalytic CO2 Methanation.

The integration of oxidation and reduction half-reactions to amplify their synergy presents a considerable challenge in CO2 photoconversion. Addressing this challenge requires the construction of spatially adjacent redox sites while suppressing charge recombination at these sites. This study introduces an innovative approach that utilizes spatial synergy to enable synergistic redox reactions within atomic proximity and employs spin polarization to inhibit charge recombination. We incorporate Mn into Co3O4 as a catalyst, in which Mn sites tend to enrich holes as water activation sites, while adjacent Co sites preferentially capture electrons to activate CO2, forming a spatial synergy. The direct H transfer from H2O at Mn sites facilitates the formation of *COOH on adjacent Co sites with remarkably favorable thermodynamic energy. Notably, the incorporation of Mn induces spin polarization in the system, significantly suppressing the recombination of photogenerated charges at redox sites. This effect is further enhanced by applying an external magnetic field. By synergizing spatial synergy and spin polarization, Mn/Co3O4 exhibits a CH4 production rate of 23.4 μmol g-1 h-1 from CO2 photoreduction, showcasing a 28.8 times enhancement over Co3O4. This study first introduces spin polarization to address charge recombination issues at spatially adjacent redox sites, offering novel insights for synergistic redox photocatalytic systems.

Antiferromagnetic magnonic charge current generation via ultrafast optical excitation

Néel spin-orbit torque allows a charge current pulse to efficiently manipulate the Néel vector in antiferromagnets, which offers a unique opportunity for ultrahigh density information storage with high speed. However, the reciprocal process of Néel spin-orbit torque, the generation of ultrafast charge current in antiferromagnets has not been demonstrated. Here, we show the experimental observation of charge current generation in antiferromagnetic metallic Mn2Au thin films using ultrafast optical excitation. The ultrafast laser pulse excites antiferromagnetic magnons, resulting in instantaneous non-equilibrium spin polarization at the antiferromagnetic spin sublattices with broken spatial symmetry. Then the charge current is generated directly via spin-orbit fields at the two sublattices, which is termed as the reciprocal phenomenon of Néel spin-orbit torque, and the associated THz emission can be detected at room temperature. Besides the fundamental significance on the Onsager reciprocity, the observed magnonic charge current generation in antiferromagnet would advance the development of antiferromagnetic THz emitter.

Giant Spin-Orbit Torque in Antiferromagnetic-Coupled Pt/[Co/Gd]N Multilayers with Suppressed Spin Dephasing and Robust Thermal Stability.

Manipulating magnetization via power-efficient spin-orbit torque (SOT) has garnered significant attention in the field of spin-based memory and logic devices. However, the damping-like SOT efficiency (ξDL) in heavy metal (HM)/ferromagnetic metal (FM) bilayers is relatively small due to the strong spin dephasing accompanied by additional spin polarization decay. Furthermore, the perpendicular magnetic anisotropy (PMA) originating from the HM/FM interface is constrained by the thickness of FM, which is unfavorable for thermal stability in practical applications. Consequently, it is valuable to develop systems that not only exhibit large ξDL but also balance thermal stability. In this work, we designed antiferromagnetic-coupled [Co/Gd]N multilayers, where staggered Co and Gd magnetic moments effectively suppress the spin dephasing and additional spin polarization decay. The ordered Co-Gd arrangements along the out-of-plane direction provide bulk PMA, endowing Pt/[Co/Gd]N high thermal stability. The SOT of Pt/[Co/Gd]N was systematically studied with N, demonstrating a significantly large ξDL of up to 0.66. The ξDL of Pt/[Co/Gd]N is greater than those of Pt/Co and Pt/ferrimagnetic alloys. This significant enhancement relies on the effective suppression of spin dephasing in [Co/Gd]N. Our work highlights that the antiferromagnetic-coupled [Co/Gd]N multilayer is a promising candidate for low-consumption and high-density spintronic devices.