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The interactions between the electronic magnetic moment and the nuclear spin moment, i.e., magnetic hyperfine (HF) interactions, play an important role in understanding electronic properties of magnetic systems and in realizing platforms for quantum information science applications. We investigate the HF interactions for atomic systems and small molecules, including Ti or Mn, by using Fermi–Löwdin orbital (FLO) based self-interaction corrected (SIC) density-functional theory. We calculate the Fermi contact (FC) and spin-dipole terms for the systems within the local density approximation (LDA) in the FLO-SIC method and compare them with the corresponding values without SIC within the LDA and generalized-gradient approximation (GGA), as well as experimental data. For the moderately heavy atomic systems (atomic number Z ≤ 25), we find that the mean absolute error of the FLO-SIC FC term is about 27 MHz (percentage error is 6.4%), while that of the LDA and GGA results is almost double that. Therefore, in this case, the FLO-SIC results are in better agreement with the experimental data. For the non-transition-metal molecules, the FLO-SIC FC term has the mean absolute error of 68 MHz, which is comparable to both the LDA and GGA results without SIC. For the seven transition-metal-based molecules, the FLO-SIC mean absolute error is 59 MHz, whereas the corresponding LDA and GGA errors are 101 and 82 MHz, respectively. Therefore, for the transition-metal-based molecules, the FLO-SIC FC term agrees better with experiment than the LDA and GGA results. We observe that the FC term from the FLO-SIC calculation is not necessarily larger than that from the LDA or GGA for all the considered systems due to the core spin polarization, in contrast to the expectation that SIC would increase the spin density near atomic nuclei, leading to larger FC terms. [ABSTRACT FROM AUTHOR]

Magnetic materials with high negative spin polarization have been sought as a building block to increase the design freedom and performance of spintronics devices. In this paper, we investigate negative spin polarization of Mn2VGa Heusler alloy in current-perpendicular-to-plane giant magnetoresistance (CPP-GMR) devices. We fabricated an epitaxial CPP-GMR stack consisting of Mn2VGa/Ag/CoFe with L21 ordering in the Mn2VGa layer and observed negative magnetoresistance (MR), which provided evidence of negative spin polarization. The MR ratio depended on thermal treatments (deposition at an elevated temperature and post-annealing), because these processes affected the ordering, roughness, and magnetic properties of Mn2VGa. The maximum MR ratio reached −1.8% at room temperature and −3.0% at low temperatures, representing the highest among the negative MR values in pseudo-spin-valve CPP-GMR devices despite the underestimation due to an incomplete antiparallel magnetization configuration. These findings demonstrate the potential of Mn2VGa for a material with high negative spin polarization. [ABSTRACT FROM AUTHOR]

Understanding the electronic transport properties of low-dimensional devices has increased dramatically in recent decades, especially for those with a promising future for application in nanotechnology. Among these nanoscopic systems are molecular systems, particularly organic molecules such as catechol, representing the small piece of a potential conductor assembled through larger biomolecules and inserted between two or more metal contacts. In this work, we present a theoretical description of the electronic transport of catechol, based on its π -conjugated aromatic system, under an external magnetic field stimulus, which is transverse to the alignment of the molecule. Thus, we analyze catechol's spintronic properties through the magnetoresistance generated by this field. We model the molecule using a tight-binding Hamiltonian and Green's functions; the transmission probability is calculated by means of the Fisher-Lee relation, and the characteristic current–voltage, spin polarization, and magnetoresistance curves based on Landauer's approach for two linking models of catechol to the metallic contacts. The results suggest a strong dependence on the spin direction of the charge carriers and the Zeeman energy (E z) on the Fermi level, generating a switch-like mechanism going from conducting to semiconducting material. This behavior opens a potential application of these catechol-based systems in future spintronic devices. [ABSTRACT FROM AUTHOR]

Chiral molecules can exhibit strong spin–orbit coupling, which can result in a large spin polarization. This is due to the fact that the energy levels of the electrons in a chiral molecule are strongly influenced by the chiral structure of the molecule, which can result in the separation of the energy levels for electrons with different spin orientations. We report a controlled spin-selective transmission of electrons through 20 base-paired poly-cytosine molecules functionalized with MoS2 flakes on ITO glass via the quantum mechanical tunneling effect. A reversion in spin polarization was observed after the silver ions interact with poly-cytosine due to the strong coordination of Ag(I) with cytosine–cytosine (C–C) mismatches, indicating the formation of duplex structural motifs, as confirmed by the circular dichroism spectroscopy at room temperature. Manipulating the spin of an electron through such a small molecule merely controlled by special cations could pave the way for major advances in spin-independent charge transport, advanced bioanalytical system design, and related applications. [ABSTRACT FROM AUTHOR]

We theoretically study the magnetic phase transition of condensed exciton-polariton microcavities in an applied magnetic field. When the magnetic field is strong, all polariton spins are polarized parallel to the magnetic field as usual. On the contrary, in the weak magnetic-field region, the polariton polarization degree is negative, namely, anti-parallel to the magnetic field. For a strong magnetic field, the magnetic phase of the polaritons arises and leads to a paramagnetic, while around a weak magnetic field, with zero exciton–photon detunings, and weak Rabi splitting the spin polarization of the polaritons leads to a diamagnetic. Thus, magneto-polariton phase transition polarization originates from the competition between the polariton Zeeman effect and polariton–polariton interactions. Moreover, the polariton polarization strongly depends on the exciton–photon detuning and Rabi splitting and has a large negative value as they are both small. At last, we compare our theoretical results with the experiments and find they match each other very well. [ABSTRACT FROM AUTHOR]

Chiral molecules can exhibit strong spin–orbit coupling, which can result in a large spin polarization. This is due to the fact that the energy levels of the electrons in a chiral molecule are strongly influenced by the chiral structure of the molecule, which can result in the separation of the energy levels for electrons with different spin orientations. We report a controlled spin-selective transmission of electrons through 20 base-paired poly-cytosine molecules functionalized with MoS2 flakes on ITO glass via the quantum mechanical tunneling effect. A reversion in spin polarization was observed after the silver ions interact with poly-cytosine due to the strong coordination of Ag(I) with cytosine–cytosine (C–C) mismatches, indicating the formation of duplex structural motifs, as confirmed by the circular dichroism spectroscopy at room temperature. Manipulating the spin of an electron through such a small molecule merely controlled by special cations could pave the way for major advances in spin-independent charge transport, advanced bioanalytical system design, and related applications. [ABSTRACT FROM AUTHOR]

In connection to the chiral-induced spin selectivity effect, we theoretically analyze the electronic and spin states of edges of a finite p-orbital helical atomic chain with the intra-atomic spin–orbit interaction. This model can host the spin-filtering state in which two up-spins propagate in one direction and two down-spins propagate in the opposite direction without breaking the time-reversal symmetry (TRS). The enhancement of charge modulations concentrated at the edges due to the evanescent states is induced, although the spin density is absent because of the TRS. A Zeeman field at an edge of the atomic chain, which breaks the TRS, yields a finite spin polarization, whose direction depends on the chirality of the molecule. The chirality change induces a reasonable amount of the energy difference, which may provide an insight into the enantioselective adsorption of chiral molecules on the ferromagnetic surface. [ABSTRACT FROM AUTHOR]

Enantio-discrimination and spin-dependent electrochemistry (SDE), as a manifestation of the chirality-induced spin selectivity (CISS) effect, are important phenomena that can be probed by "chiral" electrochemistry. Here, we prepared chiralized surfaces of gold and nickel, to serve as working electrodes, through effective chemisorption of enantiopure dimethyl-bis(ethylenedithio)-tetrathiafulvalene (DM-BEDT-TTF) 1, tetramethyl-bis(ethylenedithio)-tetrathiafulvalene (TM-BEDT-TTF) 2, and their capped silver nanoparticle (AgNPs) aggregate by simple incubation of the metallic substrates. The effective chemisorption was checked by means of ultrahigh vacuum x-ray photoelectron spectroscopy (XPS) and by electro-desorption experiments, i.e., cyclic voltammetry (CV) scans showing a first electro-desorption peak at about −1.0 V. The Au|1 and Au|2 chiral electrodes were successfully used in CV experiments exploiting chiral redox probes. Finally, the hybrid interfaces Ni|enantiopure 1 or 2|AgNPs served as working electrodes in SDE experiments. In particular, the hybrid chiral interfaces Ni|(R)-2|AgNPs and Ni|(S)-2|AgNPs exhibited a significant spin-filtering ability, as a manifestation of the CISS effect, with average spin polarization values of 15%. [ABSTRACT FROM AUTHOR]

In this paper, we investigated the spin transport properties of binuclear manganese phthalocyanine (M n 2 P c 2) spintronic devices sandwiched between two nickel electrodes using the non-equilibrium Green's function method in combination with density functional theory. Based on the calculation results, the M n 2 P c 2 device exhibited excellent spin-filtering capabilities, demonstrating an exceptionally high spin filter efficiency (SFE). Irrespective of the parallel or antiparallel orientation of magnetization in the electrodes, we observed that when both manganese atoms were in a spin-up state, the SFE of spin-resolved currents under finite bias and the thermoelectric currents induced by temperature gradients at fixed temperatures were both close to 100%. The large spin Seebeck polarization of the M n 2 P c 2 device was also obtained at low reference temperatures. This study explores the potential for developing multifunctional spintronic single-molecule devices using Ni − M n 2 P c 2. [ABSTRACT FROM AUTHOR]

The article discusses the chiral induced spin selectivity effect (CISS), which is the finding that the motion of an electron within or through chiral systems depends on the spin of that electron. The article explains that while the effect has been observed experimentally, developing a quantitative theoretical description has been challenging. The article also highlights the different types of experimental measurements that have been used to study CISS, including measurements of spin-dependent transmission, tunneling currents, magnetization, and magnetic domains. The article concludes by discussing the potential applications of CISS in spintronics, electrochemistry, and biology, and expresses optimism that further research will reveal the mechanism behind the CISS effect. [Extracted from the article]

We report on a strategy to indirectly read out the spectrum of an electronic spin via polarization transfer to nuclear spins in its local environment. The nuclear spins are far more abundant and have longer lifetimes, allowing for repeated polarization accumulation in them. Subsequent nuclear interrogation can reveal information about the electronic spectral density of states. We experimentally demonstrate the method by reading out the ESR spectrum of nitrogen vacancy center electrons in diamond via readout of lattice 13C nuclei. Spin-lock control on the 13C nuclei yields a significantly enhanced signal-to-noise ratio for the nuclear readout. Spectrally mapped readout presents operational advantages in being background-free and immune to crystal orientation and optical scattering. We harness these advantages to demonstrate applications in underwater magnetometry. The physical basis for the "one-to-many" spectral map is itself intriguing. To uncover its origin, we develop a theoretical model that maps the system dynamics, involving traversal of a cascaded structure of Landau–Zener anti-crossings, to the operation of a tilted "Galton board." This work points to new opportunities for "ESR-via-NMR" in dilute electronic systems and in hybrid electron–nuclear quantum memories and sensors. [ABSTRACT FROM AUTHOR]

Chiral molecules can act as spin filters, preferentially transmitting electrons with spins polarized along their direction of travel, an effect known as chirality-induced spin selectivity (CISS). In a typical experiment, injected electrons tunnel coherently through a layer of chiral material and emerge spin-polarized. It is also possible that spin polarization arises in radical pairs formed photochemically when electrons hop incoherently between donor and acceptor sites. Here we aim to identify the magnetic properties that would optimise the visibility of CISS polarization in time-resolved electron paramagnetic resonance (EPR) spectra of transient radical pairs without the need to orient or align their precursors. By simulating spectra of actual and model systems, we find that CISS contributions to the polarization should be most obvious when at least one of the radicals has small g-anisotropy and an inhomogeneous linewidth larger than the dipolar coupling of the two radicals. Under these conditions there is extensive cancellation of absorptive and emissive enhancements making the spectrum sensitive to small changes in the individual EPR line intensities. Although these cancellation effects are more pronounced at lower spectrometer frequencies, the spectral changes are easier to appreciate with the enhanced resolution afforded by high-frequency EPR. Consideration of published spectra of light-induced radical pairs in photosynthetic bacterial reaction centres reveals no significant CISS component in the polarization generated by the conventional spin-correlated radical pair mechanism. [ABSTRACT FROM AUTHOR]

We present computational results on electronic, magnetic, and structural properties of CoVMnSb, a quaternary Heusler alloy. Our calculations indicate that this material may crystallize in two energetically close structural phases: inverted and regular cubic. The inverted cubic phase is the ground state, with ferrimagnetic alignment, and around 80% spin polarization. Despite having a relatively large bandgap in the minority-spin channel close to the Fermi level, this phase does not undergo a half-metallic transition under pressure. This is explained by the "pinning" of the Fermi level at the minority-spin states at the Γ point. At the same time, the regular cubic phase is half-metallic and retains its perfect spin polarization under a wide range of mechanical strain. Transition to a regular cubic phase may be attained by applying uniform pressure (but not biaxial strain). In practice, this pressure may be realized by an atomic substitution of non-magnetic atoms (Sb) with another non-magnetic atom (Si) of a smaller radius. Our calculations indicate that 25% substitution of Sb with Si results in a half-metallic regular cubic phase being the ground state. In addition, CoVMnSb0.5Si0.5 retains its half-metallic properties under a considerable range of mechanical pressure, as well as exhibits thermodynamic stability, thus making this alloy attractive for potential spintronic applications. We hope that the presented results will stimulate experimental efforts to synthesize this compound. [ABSTRACT FROM AUTHOR]

Mastering the manipulation of the electron spin plays a crucial role in comprehending the behavior of organic materials in several applications, such as asymmetric catalysis, chiroptical switches, and electronic devices. A promising avenue for achieving such precise control lies in the Chiral Induced Spin Selectivity (CISS) effect, where electrons with a favored spin exhibit preferential transport through chiral assemblies of specific handedness. Chiral supramolecular polymers emerge as excellent candidates for exploring the CISS effect due to their ability to modulate their helical structure through noncovalent interactions. In this context, systems capable of responding to external stimuli are particularly intriguing, sometimes even displaying chirality inversion. This study unveils spin selectivity in chiral supramolecular polymers, derived from single enantiomers, through scanning tunneling microscopy conducted in scanning tunneling spectroscopy mode. Following two distinct sample preparation protocols for each enantiomer, we generate supramolecular polymers with opposite handedness and specific spin transport characteristics. Our primary focus centers on chiral π-conjugated building blocks, with the aim of advancing novel systems that can inspire the organic spintronics community from a supramolecular chemistry level. [ABSTRACT FROM AUTHOR]

A gold surface is functionalized by chemisorption of the enantiopure N,N′-bis-[2,2′;5′,2″]tert-thiophene-5-yl methylcyclohexane-1,2-diamine (2T3N), a chiral oligothiophene derivative, via overnight incubation in a 2T3N ethanol solution. The Au|2T3N interface is characterized by x-ray photoelectron circular dichroism and comparing x-ray photoemission spectroscopy and electro-desorption results. Charge transmission at the Au|2T3N| solution interface is characterized by recording the cyclic voltammetry of the Fe(III)/Fe(II) reversible redox couple, finding a charge transfer rate constant, k°, variation from 1 × 10−1 to 3.3 × 10−2 cm s−1, when comparing the bare Au and the Au|2T3N interfaces, respectively. The "anomalous" high value of k° found for the chiral Au|2T3N interface can be rationalized on the basis of the chiral-induced spin selectivity effect, as further proved by magnetic–conductive atomic force microscopy measurements at room temperature. A spin polarization of about 30% is found. [ABSTRACT FROM AUTHOR]

Organic solar cells (OSCs) have emerged as a promising technology for renewable energy generation due to their low cost, lightweight, flexibility, and compatibility with roll-to-roll manufacturing. However, OSCs still face challenges in achieving high power conversion efficiency (PCE) due to various factors, including recombination loss. In this study, we investigated the effect of introducing a layer of eight atomic percent gadolinium-doped zinc oxide (Zn0.92Gd0.08O) between the poly(3-hexylthiophene) (P3HT): [6,6]-phenyl butyric acid methyl ester (PCBM) active layer and the fluorine-doped tin oxide (FTO) electrode of the OSC. The reference cell, which has an Au/P3HT:PCBM/ZnO/FTO structure, exhibits a PCE of 0.52%. Remarkably, when the Zn0.92Gd0.08O layer was inserted (Au/P3HT:PCBM/Zn0.92Gd0.08O/FTO), the PCE increased significantly to 3.42%, which is more than six times the increase. Through further analysis, we present that the insertion of the Zn0.92Gd0.08O layer induces spin polarization in the P3HT:PCBM layer, leading to enhanced charge transport and reducing the recombination rate. Based on the findings, it can be concluded that the Zn0.92Gd0.08O film can potentially improve OSC performance. [ABSTRACT FROM AUTHOR]

Electron transport through a variety of helical structures has been shown to exhibit high-efficiency spin filtering, which is called chirality-induced spin selectivity (CISS). In this paper, we consider a helical chain of atomic p orbitals, which has been employed as a model in exploring the mechanism of CISS in previous theories, and show that the interatomic hopping along the helical chain induces an effective magnetic field (EMF) acting on the atomic orbital angular momentum (OAM). In chains where the curvature and torsion of the helix are small, we find that the EMF on the binormal component of the atomic OAM is created by the curvature, while that on the tangential component is produced by the torsion. We show that such coupling of the atomic OAM and the interatomic hopping leads to current-induced orbital and spin polarizations. We expect that the present coupling, which is expressed locally, can be used to estimate orbital and spin polarizations locally induced in molecules and solids. [ABSTRACT FROM AUTHOR]

Nonlocal spin polarization phenomena are thoroughly investigated in the devices made of chiral metallic single crystals of CrNb3S6 and NbSi2 as well as of polycrystalline NbSi2. We demonstrate that simultaneous injection of charge currents in the opposite ends of the device with the nonlocal setup induces the switching behavior of spin polarization in a controllable manner. Such a nonlocal spin polarization appears regardless of the difference in the materials and device dimensions, implying that the current injection in the nonlocal configuration splits spin-dependent chemical potentials throughout the chiral crystal even though the current is injected into only a part of the crystal. We show that the proposed model of the spin dependent chemical potentials explains the experimental data successfully. The nonlocal double-injection device may offer significant potential to control the spin polarization to large areas because of the nature of long-range nonlocal spin polarization in chiral materials. [ABSTRACT FROM AUTHOR]

The control of electron spin, crucial to the stability of matter, offers new possibilities for manipulating the properties of molecules and materials with potential applications in spintronics and chemical reactions. Recent experiments have demonstrated that electron transmission through chiral molecules depends on the electron spin orientation, a phenomenon known as chiral-induced spin selectivity (CISS). In this study, we show that CISS can be observed in achiral systems driven by an external circularly polarized laser field in the framework of Floquet engineering. By using the Floquet theory for a time-periodically driven system to investigate spin-dependent electron transport in a two-terminal setup, we demonstrate that the spin polarization can approach unity if the light intensity is sufficiently strong, the rate of dephasing is sufficiently low, and the average chemical potential of the two leads is within an appropriate range of values, which is narrow because of the high frequency of the laser field. To obtain a broader range of energies for large spin polarization, a combination of chiral molecules and light–matter interactions is considered, and the spin polarization of electrons transported through a helical molecule driven by a laser field is evaluated. [ABSTRACT FROM AUTHOR]

It has been demonstrated previously that electrons interact differently with chiral molecules depending on their polarization. For enantiomeric pure monolayers of heptahelicene, opposite asymmetries in spin polarization were reported and attributed to the so-called chirality-induced spin selectivity effect. However, these promising proof-of-concept photoemission experiments lack the angular and energy resolution that could provide the necessary insights into the mechanism of this phenomenon. In order to fill in the missing gaps, we provide a detailed spin- and angle-resolved photoemission spectroscopy study of heptahelicene layers on a Cu(111) substrate. Throughout the large accessible energy and angle range, no chirality induced spin asymmetry in photoemission could be observed. Possible reasons for the absence of signatures of the spin-dependent electron transmission through the chiral molecular layer are briefly discussed. [ABSTRACT FROM AUTHOR]

Bio-spinterfaces present numerous opportunities to study spintronics across the biomolecules attached to (ferro)magnetic electrodes. While it offers various exciting phenomena to investigate, it is simultaneously challenging to make stable bio-spinterfaces as biomolecules are sensitive to many factors that it encounters during thin-film growth to device fabrication. The chirality-induced spin-selectivity effect is an exciting discovery, demonstrating an understanding that a specific electron's spin (either up or down) passes through a chiral molecule. The present work utilizes Ustilago maydis Rvb2 protein, an ATP-dependent DNA helicase (also known as Reptin), to fabricate bio-spintronic devices to investigate spin-selective electron transport through the protein. Ferromagnetic materials are well-known for exhibiting spin-polarization, which many chiral and biomolecules can mimic. We report herein spin-selective electron transmission through Rvb2 that exhibits 30% spin polarization at a low bias (+0.5 V) in a device configuration, Ni/Rvb2 protein/indium tin oxide measured under two different magnetic configurations. Our findings demonstrate that biomolecules can be put in circuit components without any expensive vacuum deposition for the top contact. The present study holds a remarkable potential to advance spin-selective electron transport in other biomolecules, such as proteins and peptides, for biomedical applications. [ABSTRACT FROM AUTHOR]

Different from conventional ferromagnetic methods, producing a spin-polarized current through electrical ways in spintronic devices can greatly increase operating speed, reduce power consumption, and improve device integration. Inspired by recent experimental progress on the synthesis of a heptauthrene molecule, we investigate its spin-dependent transport contacted with Au electrodes through first-principles calculations. By applying a gate voltage, the transmission can be switched between completely spin-up and spin-down polarized states, achieving an electrically controlled dual-spin filter. Furthermore, a fine tuning on the spin polarization, between 100% and − 100%, can also be realized, where the transport with any ratio of spin-up to spin-down electron quantities can be realized beyond the traditional devices. The peculiar transmission spectra and their shift are found to play crucial roles, where transmission peaks distribute on both sides of the Fermi level with opposite spin components. Such a spin-polarization modulating effect is found to be robust to the molecule-electrode contacting site, indicating it is an intrinsic feature of such systems. Moreover, the dimension of the device is at the single-molecule level, suggesting great application potential. [ABSTRACT FROM AUTHOR]

Second-order Møller-Plesset perturbation theory (MP2) often breaks down catastrophically in small-gap systems, leaving much to be desired in its performance for myriad chemical applications such as noncovalent interactions, thermochemistry, and dative bonding in transition metal complexes. This divergence problem has reignited interest in Brillouin-Wigner perturbation theory (BWPT), which is regular at all orders but lacks size consistency and extensivity, severely limiting its application to chemistry. In this work, we propose an alternative partitioning of the Hamiltonian that leads to a regular BWPT perturbation series that, through the second order, is size-extensive, size-consistent (provided its Hartree–Fock reference is also), and orbital invariant. Our second-order size-consistent Brillouin-Wigner (BW-s2) approach can describe the exact dissociation limit of H2 in a minimal basis set, regardless of the spin polarization of the reference orbitals. More broadly, we find that BW-s2 offers improvements relative to MP2 for covalent bond breaking, noncovalent interaction energies, and metal/organic reaction energies, although rivaling coupled-cluster with single and double substitutions for thermochemical properties. [ABSTRACT FROM AUTHOR]

The theory of the magnetic coupling between the localized spins, mediated by the mobile excess electron, is generalized to the case of a trigonal, six-center, four-electron molecule with partial valence delocalization. The combination of the electron transfer occurring within the valence-delocalized subsystem and the interatomic exchange producing coupling of the spin of the mobile electron of valence-delocalized fragment with the three localized spins forming the valence-localized subsystem leads to the appearance of a special kind of double exchange (DE), termed the "external core double exchange" (ECDE), in order to distinguish such DE from the conventional "internal core double exchange" for which the mobile electron is coupled with the spin-cores on the same center via the intra-atomic exchange. The effect of the ECDE on the ground spin state of the considered trigonal molecule is compared with earlier reported effect produced by DE in the four-electron, mixed-valence (MV) trimer. A high diversity of the ground spin states is revealed, depending on the relative magnitudes and signs of the electron transfer and interatomic exchange parameters, with part of these states not appearing to be the ground states in a trigonal trimer exhibiting DE. We briefly discuss some examples of trigonal MV systems from the point of view of the possibility to have different combinations of signs of the transfer and exchange parameters and, accordingly, different ground spin states. The tentative role of the considered systems in molecular electronics and spintronics is also noticed. [ABSTRACT FROM AUTHOR]

In this paper, we outline a physically motivated framework for describing spin-selective recombination processes in chiral systems, from which we derive spin-selective reaction operators for recombination reactions of donor–bridge–acceptor molecules, where the electron transfer is mediated by chirality and spin–orbit coupling. In general, the recombination process is selective only for spin-coherence between singlet and triplet states, and it is not, in general, selective for spin polarization. We find that spin polarization selectivity only arises in hopping-mediated electron transfer. We describe how this effective spin-polarization selectivity is a consequence of spin-polarization generated transiently in the intermediate state. The recombination process also augments the coherent spin dynamics of the charge separated state, which is found to have a significant effect on the recombination dynamics and to destroy any long-lived spin polarization. Although we only consider a simple donor–bridge–acceptor system, the framework we present here can be straightforwardly extended to describe spin-selective recombination processes in more complex systems. [ABSTRACT FROM AUTHOR]

An experimental and computational optical pump-probe model is constructed, which utilizes two ultrafast pump pulses within the repetition period of a mode-locked laser to generate electron spin polarization. This report focuses on the effects of resonant spin amplification induced by an infinite train of the two-pump pulses. The first pump pulse is used to generate ordinary resonant spin amplification spectra, while the second pump pulse is used to manipulate the generated spectra. This model gives control of the accumulation of spin polarized electrons along a magnetic field by selecting the temporal separation of the two-pump pulses. The computational model accurately predicts and agrees with the experimental results, which shows manipulation of resonant spin peaks that are no longer entirely dependent on the external magnetic field. This two-pump model and the associated manipulations of resonant spin peaks can be used as a platform to construct and conceptualize resonant spin amplification-based optospintronic devices and applications. [ABSTRACT FROM AUTHOR]

The Goos–Hänchen (GH) shift and the spin polarization are theoretically investigated under the anti-parallel double δ -magnetic-barrier nanostructure model by applying a bias using Airy's function formalism and transfer-matrix technique, which is an improvement on previous calculation. The results show the magnitude and sign of GH shift and spin polarization can be easily changed by modulating the applied bias. The closer the applied bias to the critical value is, the more intensive GH shift and spin polarization will be. Furthermore, two critical values come through modulating the strength of magnetic fields, and an intensive GH shift and a spin polarization also exist near each critical value. These findings can provide a practical approach to designing and fabricating spin beam filters or splitters modulated by applied bias. [ABSTRACT FROM AUTHOR]

The document is a contents list for the journal "Chemical Communications" published in 2024. It includes various articles and communications on topics such as heterogeneous catalytic activity, 3D printing of soft active materials, synthesis of substituted a-carbolines, and the structure of caffeine-pyrogallol complex. The journal is published by The Royal Society of Chemistry, a leading chemistry community. The document also mentions approved training courses offered by the society. [Extracted from the article]

In recent years, there has been significant attention towards the development of catalysts that exhibit superior performance and environmentally friendly attributes. This surge in interest is driven by the growing demands for energy utilization and storage as well as environmental preservation. Spin polarization plays a crucial role in catalyst design, comprehension of catalytic mechanisms, and reaction control, offering novel insights for the design of highly efficient catalysts. However, there are still some significant research gaps in the current study of spin catalysis. Therefore, it is urgent to understand how spin polarization impacts catalytic reactions to develop superior performance catalysts. Herein, we present a comprehensive summary of the application of spin polarization in catalysis. Firstly, we summarize the fundamental mechanism of spin polarization in catalytic reactions from two aspects of kinetics and thermodynamics. Additionally, we review the regulation mechanism of spin polarization in various catalytic applications and several approaches to modulate spin polarization. Moreover, we discuss the future development of spin polarization in catalysis and propose several potential avenues for further progress. We aim to improve current catalytic systems through implementing a novel and distinctive spin engineering strategy. [ABSTRACT FROM AUTHOR]

The inherently low spin polarization of ferromagnetism in two-dimensional C3N hinders its application in spintronics. Addressing this, the impact of (V, Cu) co-doping on the spin polarization in monolayer C3N has been systemically explored through first-principles calculations. The results reveal that doping with a single V or Cu atom at an N site significantly enhances spin polarization compared to doping at a C site. Moreover, substituting a single C or N atom with a V atom results in significantly enhanced spin polarization compared to replacement with a Cu atom. Significantly, V and Cu co-doping at different N sites in C3N systems uniformly favors ferromagnetic states. A remarkable boost in spin polarization is achieved through strategic co-doping of V and Cu at N sites, separated by a distance of 5.681 Å. This enhancement is attributed to the coupling interactions among the C 2p, N 2p, Cu 3d, and V 3d orbitals. The theoretical investigation suggests an effective route to greatly enhance the spin polarization through targeted 3d transition metal co-doping, contributing to the development of high-performance spintronic devices and advancing quantum computing technologies. [ABSTRACT FROM AUTHOR]

The investigation into approaches for achieving reversible control of topological phase transitions has attracted substantial research interest. So far, several system‐dependent physical control methods are developed, while a chemical strategy for efficient regulation of topological properties is still lack. Here, this study presents a chemical means to achieve reversible topological control in 2D organometallic lattices by introducing the lactam‐lactim tautomerization modules in the organic linkers. The strategy is validated in the theoretically designed 2D hexagonal framework with planar tricoordinated Co as nodes and 2,2′‐bithiazole derivatives as organic linkers, which transforms from a ferrimagnetic half metal with a local gap featuring Chern number of +1 to a ferromagnetic Chern insulator possessing Chern number of −1 after lactam‐lactim tautomerization. Simultaneously, a flip in the spin polarization of charge carriers between the two lattice tautomers is also observed. [ABSTRACT FROM AUTHOR]

The single‐atom Fe−N−C catalyst has shown great promise for the oxygen reduction reaction (ORR), yet the intrinsic activity is not satisfactory. There is a pressing need to gain a deeper understanding of the charge configuration of the Fe−N−C catalyst and to develop rational modulation strategies. Herein, we have prepared a single‐atom Fe catalyst with the co‐coordination of N and O (denoted as Fe−N/O−C) and adjacent defect, proposing a strategy to optimize the d‐orbital spin‐electron filling of Fe sites by fine‐tuning the first coordination shell. The Fe−N/O−C exhibits significantly better ORR activity compared to its Fe−N−C counterpart and commercial Pt/C, with a much more positive half‐wave potential (0.927 V) and higher kinetic current density. Moreover, using the Fe−N/O−C catalyst, the Zn‐air battery and proton exchange membrane fuel cell achieve peak power densities of up to 490 and 1179 mW cm−2, respectively. Theoretical studies and in situ electrochemical Raman spectroscopy reveal that Fe−N/O−C undergoes charge redistribution and negative shifting of the d‐band center compared to Fe−N−C, thus optimizing the adsorption free energy of ORR intermediates. This work demonstrates the feasibility of introducing an asymmetric first coordination shell for single‐atom catalysts and provides a new optimization direction for their practical application. [ABSTRACT FROM AUTHOR]

Context: The coherent electron/spin transport in azurin, a species of copper protein, was calculated based on the Landauer model. The research is motivated by the fast electron transport and spin selectivity/polarization in azurin, which have been reported in relation to the chiral-induced spin selectivity of the peptide structure. The calculated spin polarization of copper proteins was large. This phenomenon was strongly influenced by the spin density of the atoms in the ligand group, whereas the contribution of copper was negligible. The results suggest that spin polarization in copper proteins is enhanced by that of the ligand groups. The predicted spin polarization aligns primarily with the scanning tunneling microscope-based break-junction technique to study the electronic properties of single-molecule junctions. Methods: Computational techniques employed in this study are nonequilibrium Green's functions (NEGF) and density functional theory (DFT) based on the Landauer model, implemented using the QuantumATK software (Synopsys Inc.). The Perdew-Burke-Ernzerhof (PBE) exchange-correlation functional was adopted for spin-polarized generalized gradient approximation (SGGA). The valence atomic orbitals were constructed using the wavefunctions of the SIESTA package, which was based on the norm-conserving Troullier–Martins relativistic pseudopotentials for describing core electrons. The mesh used for real-space integration was 150 Ha. [ABSTRACT FROM AUTHOR]

Understanding 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. [ABSTRACT FROM AUTHOR]

This research aims to employ a first-principles approach based on density functional theory (DFT) to predict the structural, electronic, and magnetic attributes of CdMX compounds, where M represents Ru , Rh , or Pd , and X represents either S or Se . We utilized the modified Beck-Johnson potential, combined with the generalized gradient approximation ( mBJGGA ), to scrutinize the electronic and magnetic features of these compounds. The results reveal robust magnetic ground states for M -doped CdX . The analysis of spin-polarized band structures and densities of states indicates that CdRuX and CdPdX compounds exhibit half-metallic ferromagnetism, characterized by complete spin polarization of 100% at the Fermi level. Conversely, CdRhX compounds exhibit the properties of ferromagnetic semiconductors. For Ru , Rh , and Pd -doped CdX , an integer-integrated total magnetic moment is observed, corresponding to 4, 3, and 2 μ B , respectively, with the primary contribution stemming from the doping atom and its four nearest neighboring X atoms. This ferromagnetic behavior is attributed to the strong p - d hybridization occurring between the states of the host X ions and the M impurity ion. Consequently, the outcomes of our study render these alloys as suitable materials for possible spintronic devices. [ABSTRACT FROM AUTHOR]

Recently, the altermagnetic materials with spin splitting effect (SSE), have drawn significant attention due to their potential to the flexible control of the spin polarization by the Néel vector. Here, the direct and inverse altermagnetic SSE (ASSE) in the (101)‐oriented RuO2 film with the tilted Néel vector are reported. First, the spin torque along the x‐, y‐, and z‐axis is detected from the spin torque‐induced ferromagnetic resonance (ST‐FMR), and the z‐spin torque emerges when the electric current is along the [010] direction, showing the anisotropic spin splitting of RuO2. Further, the current‐induced modulation of damping is used to quantify the damping‐like torque efficiency (ξDL) in RuO2/Py, and an anisotropic ξDL is obtained and maximized for the current along the [010] direction, which increases with the reduction of the temperature, indicating the present of ASSE. Next, by way of spin pumping measurement, the inverse altermagnetic spin splitting effect (IASSE) is studied, which also shows a crystal direction‐dependent anisotropic behavior and temperature‐dependent behavior. This work gives a comprehensive study of the direct and inverse ASSE effects in the altermagnetic RuO2, inspiring future altermagnetic materials and devices with flexible control of spin polarization. [ABSTRACT FROM AUTHOR]

Recently, the altermagnetic materials with spin splitting effect (SSE), have drawn significant attention due to their potential to the flexible control of the spin polarization by the Néel vector. Here, the direct and inverse altermagnetic SSE (ASSE) in the (101)‐oriented RuO2 film with the tilted Néel vector are reported. First, the spin torque along the x‐, y‐, and z‐axis is detected from the spin torque‐induced ferromagnetic resonance (ST‐FMR), and the z‐spin torque emerges when the electric current is along the [010] direction, showing the anisotropic spin splitting of RuO2. Further, the current‐induced modulation of damping is used to quantify the damping‐like torque efficiency (ξDL) in RuO2/Py, and an anisotropic ξDL is obtained and maximized for the current along the [010] direction, which increases with the reduction of the temperature, indicating the present of ASSE. Next, by way of spin pumping measurement, the inverse altermagnetic spin splitting effect (IASSE) is studied, which also shows a crystal direction‐dependent anisotropic behavior and temperature‐dependent behavior. This work gives a comprehensive study of the direct and inverse ASSE effects in the altermagnetic RuO2, inspiring future altermagnetic materials and devices with flexible control of spin polarization. [ABSTRACT FROM AUTHOR]

Nowadays there is considerable interest in the photogalvanic effect in low-dimensional devices. In this work, we built a two-dimensional Bi2C-based photodetector and explored the spin-dependent photogalvanic effect under linearly polarized light and zero-bias conditions which can produce experimentally observable photoelectron flow. It was discovered that by introducing vacancies and substitution-doping into the Bi2C photodetector, the photogalvanic effect could be enhanced by 10–100 times that of a pristine photodetector, which is sufficient to be detected in experiments. Moreover, due to strong spin–orbit interactions, the Bi2C photodetector can produce very high spin polarization, even 100% full spin polarization, and pure spin current at a specific incident angle and photon energy, for example in the Bi1-vacancy Bi2C photodetector. In addition, the photon energy of incident light can regulate the produced spin photocurrent, which shows considerable anisotropy. Our results highlight the potential of the Bi2C photodetector as a versatile device in optoelectronics and spintronics applications. [ABSTRACT FROM AUTHOR]

Polarization has opened a new physics chapter in relativistic heavy-ion collisions. Since the first prediction and experimental observation of global spin polarization, a lot of progress has been made in understanding its features, both at experimental and theoretical levels. In this paper, we give an overview on the recent advances in this field. The covered topics include a review of measurements of global and local spin polarization of hyperons and the global spin alignment of vector meson’s. We account for the basic theoretical framework to describe spin polarization in a relativistic fluid such as the Quark–Gluon Plasma, including statistical quantum field theory and local thermodynamic equilibrium, spin hydrodynamics, relativistic kinetic theory with spin and coalescence models. [ABSTRACT FROM AUTHOR]

Rationally designing of highly efficient electrocatalysts is critical to improving hydrogen production by water electrolysis. However, bottlenecks still require consideration when optimizing the intrinsic performance of electrocatalysts. Applying appropriate external fields to catalytic systems may effectively overcome such bottlenecks and enhance the performance of catalysts. Among various external fields, the magnetic field has received extensive attention owing to its multifunctionality, non‐contact nature, and non‐invasiveness, thereby requiring more research and development. In this review, recent advances in magnetic field‐assisted water electrolysis are systematically outlined. Firstly, the diverse methods used for pre‐regulating catalysts under magnetic fields, including optimized nucleation, induction heating, and directed growth, are discussed. It then explores the effects of magnetic fields on electrochemical processes, including magnetothermal, magnetohydrodynamic, and induced electric impact. Then, the influences of magnetic fields on the intrinsic properties of catalysts, such as spin polarization and spin reconstruction effects, are addressed. Finally, a discussion of the potential perspectives of magnetic field‐enhanced water splitting, including catalyst design, experimental precision, and in situ characterization, are then provided to guide further research. [ABSTRACT FROM AUTHOR]

We performed spin-torque ferromagnetic resonance studies on the Al/NiFe/AlOx heterostructure. We observed a large non-trivial field-like torque, τ FL z , due to the out-of-plane spin polarization, despite the lack of heavy metal in our multilayer. The torque conductivity is found to be significant with a value equal to σ FL z = (21 ± 2) ℏ 2 e × 10 3 Ω − 1 m − 1 . From a detailed Al thickness dependence, we show that τ FL z arises from the interface between Al and NiFe. We demonstrate that the observed τ FL z arises from the spin-swapping mechanism at the Al/NiFe interface rather than the orbital Hall effect of Al. This observation of a non-trivial spin–orbit torque in the low-cost light element, Al, is highly significant for the energy-efficient control of spintronic devices. [ABSTRACT FROM AUTHOR]

Polar materials, with intrinsic polarization effects, present significant potential for photo(electro)catalysis. However, the available natural polar materials in this field are quite scarce, due to the requisite structural non‐centrosymmetry. Defect engineering emerges as a promising avenue for tuning material symmetry, yet achieving the transition from centrosymmetric to non‐centrosymmetric structures and optimizing associated polarization effects remains challenging. This study demonstrates symmetry breaking in centrosymmetric 3R‐delafossite AgFeO2 through ordered oxygen defects introduction, yielding substantial macroscopic polarization. The transition is achieved via annealing post‐treatment of co‐precipitation‐hydrothermal AgFeO2 samples, with precision in oxygen defects control by tailoring annealing conditions. Experimental characterizations reveal ordered interstitial oxygen and disordered oxygen vacancies. Density functional theory calculations indicate a higher propensity for the formation of disordered oxygen vacancies compared to ordered ones, while ordered interstitial oxygen is more easily formed than its disordered counterpart. Resultant macroscopic polarization enhances photoelectrochemical performance, with photocurrent density increasing from 0.79 to 2.95 µA cm−2. Coupling macroscopic and spin polarization via external electric and magnetic fields further enhances photocurrent density (≈18.44 µA cm−2). These findings provide reference cases and strategies for applying polarization effects in photo(electro)catalytic technology. [ABSTRACT FROM AUTHOR]

Efficient spin sources with large spin Hall angle (θSH) and long spin diffusion length (λSD) are highly desired in the application of spintronic devices. However, due to strong spin‐orbit coupling, the two targets can hardly be achieved simultaneously in conventional relativistic spin sources, like heavy metals. Here, it is proven that collinear antiferromagnetic RuO2 films are able to address this key issue and break the inverse relationship of θSH versus λSD. Based on spin torque‐ferromagnetic resonance and spin pumping measurements, the authors demonstrate that the θSH of RuO2(100) films is 0.183, and the λSD is over 12 nm being an order of magnitude longer than that of Pt, β‐W, and β‐Ta. Meanwhile, sizable λSD is also obtained in spin current with out‐of‐plane spin polarization generated by RuO2(101) films. By conducting a control experiment, the nonrelativistic altermagnetic spin splitting effect (ASSE) is ascertained to be the crucial mechanism accounting for the simultaneous large θSH and long λSD in RuO2. Besides the fundamental significance, these findings will advance the development of spintronics towards higher efficiency and lower power consumption. [ABSTRACT FROM AUTHOR]

[Display omitted] The efficiency of CO 2 photocatalytic reduction is severely limited by inefficient separation and sluggish transfer. In this study, spin polarization was induced and built-in electric field was strengthened via Co doping in the BiVO 4 cell to boost photocatalytic CO 2 reduction. Results showed that owing to the generation of spin-polarized electrons upon Co doping, carrier separation and photocurrent production of the Co-doped BiVO 4 were enhanced. CO production during CO 2 photocatalytic reduction from the Co-BiVO 4 was 61.6 times of the BiVO 4. Notably, application of an external magnetic field (100 mT) further boosted photocatalytic CO 2 reduction from the Co-BiVO 4 , with 68.25 folds improvement of CO production compared to pristine BiVO 4. The existence of a built-in electric field (IEF) was demonstrated through density functional theory (DFT) simulations and kelvin probe force microscopy (KPFM). Mechanism insights could be elucidated as follows: doping of magnetic Co into the BiVO 4 resulted in increased the number of spin-polarized photo-excited carriers, and application of a magnetic field led to an augmentation of intrinsic electric field due to a dipole shift, thereby extending carrier lifetime and suppressing charges recombination. Additionally, HCOO− was a crucial intermediate in the process of CO 2 RR, and possible pathways for CO 2 reduction were proposed. This study highlights the significance of built-in electric fields and the important role of spin polarization for promotion of photocatalytic CO 2 reduction. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

Efficient spin sources with large spin Hall angle (θSH) and long spin diffusion length (λSD) are highly desired in the application of spintronic devices. However, due to strong spin‐orbit coupling, the two targets can hardly be achieved simultaneously in conventional relativistic spin sources, like heavy metals. Here, it is proven that collinear antiferromagnetic RuO2 films are able to address this key issue and break the inverse relationship of θSH versus λSD. Based on spin torque‐ferromagnetic resonance and spin pumping measurements, the authors demonstrate that the θSH of RuO2(100) films is 0.183, and the λSD is over 12 nm being an order of magnitude longer than that of Pt, β‐W, and β‐Ta. Meanwhile, sizable λSD is also obtained in spin current with out‐of‐plane spin polarization generated by RuO2(101) films. By conducting a control experiment, the nonrelativistic altermagnetic spin splitting effect (ASSE) is ascertained to be the crucial mechanism accounting for the simultaneous large θSH and long λSD in RuO2. Besides the fundamental significance, these findings will advance the development of spintronics towards higher efficiency and lower power consumption. [ABSTRACT FROM AUTHOR]

Semiconductor spintronics has brought about revolutionary application prospects in future electronic devices. The tunnel junction plays a key role in achieving efficient spin injection in semiconductors. This work employed the GaN semiconductor as a room-temperature spin injection system, taking advantage of its weak spin–orbit coupling and spin scattering. By introducing a lattice-matched AlN barrier layer to improve the tunneling interface, advanced spin injection and transport were realized compared with traditional oxide barriers. The spin polarization was further improved by modulating the applied bias, and a bias-controlled tunneling enhancement mechanism was revealed. Consequently, we demonstrated a high record of spin polarization of 20.5%. This work paves a feasible route for achieving efficient spin injection and transport in GaN, which will further promote the development of room-temperature and high-performance spintronic devices. [ABSTRACT FROM AUTHOR]

A phase transition accompanied by the appearance of a spike in the longitudinal resistance of a two-dimensional electron system has been studied using the electron spin resonance near the filling factor ν = 3 in the ZnO/MgZnO heterojunction. This transition occurs when the tilt angle θ of the magnetic field is increased to some critical value θc. An analysis of the spin resonance amplitude has made it possible to demonstrate the spin nature of this phenomenon. For example, the ground state of the system on both sides of the transition has a nonzero spin polarization, which changes by several times when the phase of the system is changed. Strong spin resonance is observed both at θ < θc and at θ > θc. Surprisingly, the spin resonance at the critical angle θc has been detected in only one phase, which lies in the region of magnetic fields below the critical field Bc corresponding to the spike position in the longitudinal resistance. An increase in the magnetic field to this value leads to a decrease in the resonance amplitude and an increase in the resonance width. In the field region above Bc, the spin resonance disappears completely. Such behavior of the spin resonance is most likely due to the formation of domains with different spin polarizations in the electron system. [ABSTRACT FROM AUTHOR]

This study employs a first-principles approach to comprehensively examine the structural, electronic, optical, and magnetic properties of the thermodynamically stable scintillating double perovskite halides A 2 N a T a X 6 ( A = C s , R b ; X = C l , B r , I ). The dynamic stability of these materials were explained based on deduced phonon properties. Our analysis reveals that these compounds exhibit intriguing electronic behavior with spin polarization, demonstrating half-metallicity. In spin-up, the band gap is found to be zero, while in spin-down, it falls within the range of 3 to 4 eV with the incorporation of DFT+U corrections. Notably, the optical properties assessment highlights the exceptional UV and high-energy absorption capabilities of A 2 N a T a I 6 , making it a promising candidate for scintillation applications in particle detection. This research sheds light on the unique and versatile properties of these materials, with implications for various technological and scientific applications. [ABSTRACT FROM AUTHOR]

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%. Enhancing the efficiency of solar-driven water splitting is challenging but highly interesting. Here the authors report a dual spin-controlled 2D/3D perovskite photoelectrode that achieves 12.55% efficiency by utilizing the chiral-induced spin selectivity phenomenon. [ABSTRACT FROM AUTHOR]