Long-range Spin Research Articles

Spin effect in the ferromagnetic organic photovoltaics cells

In organic photovoltaic devices, the separation and transport of photogenerated charges play crucial roles for power conversion efficiency. Magnetic doping in organic solar cells can effectively enhance the power conversion efficiency by introducing a static magnetic field. In this study, we observed that in pure organic magnetic solar cells, the spin-polarization-induced spin scattering effect can also efficiently modulate the photocurrent in solar cells. Compared to the demagnetized state, the short-circuit current of PTB7:nw-P3HT:PCBM solar cells increased by approximately 0.3% after magnetization. The dielectric constant only increased by about 0.05%. However, above the Curie temperature 310 K, the long-range spin order in PTB7:nw-P3HT:PCBM solar cells disappears, resulting in consistent circuit currents before and after magnetization. Therefore, magnetic doping can enhance the short-circuit current in organic solar cells by weakening the spin scattering effect and enhancing the charge carrier mobility.

Designed Spin-Texture-Lattice to Control Anisotropic Magnon Transport in Antiferromagnets.

Spin waves in magnetic materials are promising information carriers for future computing technologies due to their ultra-low energy dissipation and long coherence length. Antiferromagnets are strong candidate materials due, in part, to their stability to external fields and larger group velocities. Multiferroic antiferromagnets, such as BiFeO3 (BFO), have an additional degree of freedom stemming from magnetoelectric coupling, allowing for control of the magnetic structure, and thus spin waves, with the electric field. Unfortunately, spin-wave propagation in BFO is not well understood due to the complexity of the magnetic structure. In this work, long-range spin transport is explored within an epitaxially engineered, electrically tunable, 1D magnonic crystal. A striking anisotropy is discovered in the spin transport parallel and perpendicular to the 1D crystal axis. Multiscale theory and simulation suggest that this preferential magnon conduction emerges from a combination of a population imbalance in its dispersion, as well as anisotropic structural scattering. This work provides a pathway to electrically reconfigurable magnonic crystals inantiferromagnets.

Muon g−2 , long-range muon spin force, and neutrino oscillations

Recent studies have proposed using a geocentric muon spin force to account for the (g−2)μ anomaly, with the long-range force mediator being a light axionlike particle. The mediator exhibits a CP-violating scalar coupling to nucleons and a normal derivative coupling to muons. Due to the weak symmetry, this axion inevitably couples to neutrinos, providing potential impact on neutrino oscillations. By utilizing neutrino data from BOREXINO, IceCube DeepCore, Super-Kamiokande, and SNO, we have identified that both atmospheric and solar neutrino data can impose stringent constraints on the long-range muon spin force model and the (g−2)μ parameter space. With optimized data analysis techniques and the potential from future experiments, such as JUNO, Hyper-Kamiokande, SNO+, and IceCube PINGU, there exists a promising opportunity to achieve even greater sensitivities. Indeed, neutrino oscillations offer a robust and distinctive cross-check for the model, offering stringent constraints on the (g−2)μ parameter space. Published by the American Physical Society 2024

Signatures of polarized chiral spin disproportionation in rare earth nickelates

In rare earth nickelates (RENiO3), electron-lattice coupling drives a concurrent metal-to-insulator and bond disproportionation phase transition whose microscopic origin has long been the subject of active debate. Of several proposed mechanisms, here we test the hypothesis that pairs of self-doped ligand holes spatially condense to provide local spin moments that are antiferromagnetically coupled to Ni spins. These singlet-like states provide a basis for long-range bond and spiral spin order. Using magnetic resonant X-ray scattering on NdNiO3 thin films, we observe the chiral nature of the spin-disproportionated state, with spin spirals propagating along the crystallographic (101)ortho direction. These spin spirals are found to preferentially couple to X-ray helicity, establishing the presence of a hitherto-unobserved macroscopic chirality. The presence of this chiral magnetic configuration suggests a potential multiferroic coupling between the noncollinear magnetic arrangement and improper ferroelectric behavior as observed in prior studies on NdNiO3 (101)ortho films and RENiO3 single crystals. Experimentally-constrained theoretical double-cluster calculations confirm the presence of an energetically stable spin-disproportionated state with Zhang-Rice singlet-like combinations of Ni and ligand moments.

(Invited) Manipulating the Exotic Excitons of Van Der Waals Correlated Antiferromagnet with Impurities and Size

A Van der Waals correlated antiferromagnet, metal phosphorus trichalcogenides (MPX3, M = Mn, Fe, Ni; X = S, Se), have emerged as promising candidates for next generation spintronics, and quantum information technologies. Nickel phosphorus trisulfide (NiPS3) is a most notable member of this family and has been extensively studied for its unique properties, including the emergence of an ultra-sharp photoluminescence (PL) peak at ~1.476 eV below Néel temperature of 150 Kelvin. While the highly anisotropic, linearly polarized emission of this PL peak has been shown to be directly correlated to the long-range spin order of NiPS3, its ultra-narrow linewidth of a few hundred meV has led to the speculation that it is originated from a coherent many-body exciton state. Observations of multiple phonon bounds states and formation of exciton-polaritons also creates more excitement as they present new possibilities for design and control of correlated electron systems.Aiming to achieve understanding and control of this spin-correlated exciton, we conduct temperature dependent, polarization resolved, PL studies on compounds of NiPS3 doped with different concentration of Mn (Ni1-xMnxPS3) and Se (NiPS3(1-x)Se3x). We observed systematic variation in characteristics of the spin-correlated exciton revealing their sensitive dependence on disturbance in the magnetic order of NiPS3.Next, to explore the effect of nanostructuring, we developed a novel chemical synthesis for highly crystalline NiPS3 nano flakes. We observed an activation of a new exciton state that share many exciting properties of bulk spin-correlated exciton.

(Ca0.5Mn0.5)2MnTeO6 - An Anomalously Stable High-Pressure Double Perovskite.

High pressure high temperature treatments of the composition CaMnMnTeO6 are found to yield only an A2BB'O6-type double perovskite (Ca0.5Mn0.5)2MnTeO6, rather than a AA'BB'O6 double double perovskite with A- and B- site cation order as found in analogs CaMnMnReO6 and CaMnMnWO6 with similar cation sizes. Double perovskite (Ca0.5Mn0.5)2MnTeO6 adopts a monoclinic structure in space group P21/n with a framework of highly tilted MnO6 and TeO6 octahedra enclosing disordered Ca2+ and Mn2+ cations. Magnetic measurements show that (Ca0.5Mn0.5)2MnTeO6 is a highly frustrated spin glass with a freezing transition at 5 K, and no long-range spin order is apparent by neutron diffraction at 1.6 K.

Inverse Spin-Hall Effect and Spin Swapping in Spin-Split Superconductors.

When a spin-splitting field is introduced to a thin film superconductor, the spin currents polarized along the field couples to energy currents that can only decay via inelastic scattering. We study spin and energy injection into such a superconductor where spin-orbit impurity scattering yields inverse spin-Hall and spin-swapping currents. We show that the combined presence of a spin-splitting field, superconductivity, and inelastic scattering gives rise to a strong enhancement of the ordinary inverse spin-Hall effect, as well as unique inverse spin-Hall and spin-swapping signals orders of magnitude stronger than the ordinary inverse spin-Hall signal. These can be completely controlled by the orientation of the spin-splitting field, resulting in a long-range charge and spin accumulations detectable much further from the injector than in the normal state. While the enhanced inverse spin-Hall signals offer a major improvement in spin detection sensitivity, the unique spin-swap signals can be utilized for designing devices where both the spin and current directions are controlled and altered throughout the geometry.

Muon spin relaxation and emergence of disorder-induced unconventional dynamic magnetic fluctuations in Dy2Zr2O7

The disordered pyrochlore oxide Dy2Zr2O7 shows the signatures of field-induced spin freezing with remnant zero-point spin-ice entropy at 5 kOe magnetic field. We have performed zero-field and longitudinal field Muon spin relaxation (µSR) studies on Dy2Zr2O7. Our zero field studies reveal the absence of both long-range ordering and spin freezing down to 62 mK. The µSR relaxation rate exhibits a temperature-independent plateau below 4 K, indicating a dynamic ground state of fluctuating spins similar to the well-known spin ice system Dy2Ti2O7. The low-temperature spin fluctuations persist in the longitudinal field of 20 kOe as well and show unusual field dependence of the relaxation rate, which is uncommon for a spin-liquid system. Our results, combined with the previous studies do not show any evidence of spin ice or spin glass ground state, rather point to a disorder-induced dynamic magnetic ground state in the Dy2Zr2O7 material.

Quantum spin liquid ground state in the trimer rhodate Ba4NbRh3O12

Frustrated magnets offer a plethora of exotic magnetic ground states, including quantum spin liquids (QSLs), in which enhanced quantum fluctuations prevent a long-range magnetic ordering of the strongly correlated spins down to lowest temperature. Here we have investigated the trimer based mixed valence hexagonal rhodate Ba4NbRh3O12 using a combination of dc and ac magnetization, electrical resistivity, specific heat, and muon spin rotation/relaxation (μSR) measurements. Despite the substantial antiferromagnetic exchange interactions, as evident from the Weiss temperature (θW∼−35 to −45K), among the Rh-local moments, neither long-range magnetic ordering nor spin freezing is observed down to at least 50 mK, in ac-susceptibility, specific heat, and zero-field μSR measurements (down to 0.26 K). We ascribe the absence of any magnetic transition to enhanced quantum fluctuations as a result of geometrical frustration arising out of the edge-sharing equilateral Rh-triangular network in the structure. Our longitudinal-field μSR result evidences persistent spin fluctuations down to 0.26 K, thus stabilizing a dynamic QSL ground state in Ba4NbRh3O12. Furthermore, the magnetic specific heat data at low T reveal a significant T-linear contribution plus a quadratic T dependence, which may indicate the gapless Dirac QSL phenomenology of the spinon excitations with a linear dispersion. Published by the American Physical Society 2024

Enhanced magnon transport through an amorphous magnetic insulator

Conduction of spin currents in disordered insulating antiferromagnets has recently been at the center of scientific debate with both long-range spin transport or no spin transport at all observed experimentally. In this study, ferromagnetic resonance has been used to probe the transmission of ac spin current through thin amorphous yttrium iron garnet (YIG) layers. The spin current is found to be mediated by evanescent spin waves with a penetration length four times larger than that of previous studies of amorphous YIG, even exceeding the spin penetration length of crystalline NiO. Published by the American Physical Society 2024

Phase crossover induced by dynamical many-body localization in periodically driven long-range spin systems

Phase crossover induced by dynamical many-body localization in periodically driven long-range spin systems

Signature of long-ranged spin triplets across a two-dimensional superconductor/helimagnet van der Waals interface

The combination of a superconductor with a magnetically inhomogeneous material has been established as an efficient mechanism for the generation of long-ranged spin-polarized (spin-triplet) Cooper pairs. Evidence for this mechanism, however, has been demonstrated based on studies done on thin-film multilayers, where the strong bonds existing at the interface between the superconductor and the magnetic material should in principle enhance proximity effects and strengthen any electronic correlations. Here, we fabricate devices based on van der Waals (vdW) stacks of flakes of the NbS2 combined with flakes of Cr1/3NbS2, which has a built-in magnetic inhomogeneity due to its helimagnetic spin texture at low temperatures. We find that the critical temperature of these vdW heterostructures is strongly dependent on the magnetic state of Cr1/3NbS2, whose degree of magnetic inhomogeneity can be controlled via an applied magnetic field. Our results demonstrate evidence for the generation of long-ranged spin-triplet pairs across the Cr1/3NbS2/NbS2 vdW interface. Published by the American Physical Society 2024

Tailoring Interlayer Chiral Exchange by Azimuthal Symmetry Engineering.

Recent theoretical and experimental studies of the interlayer Dzyaloshinskii-Moriya interaction (DMI) have sparked great interest in its implementation into practical magnetic random-access memory (MRAM) devices, due to its capability to mediate long-range chiral spin textures. So far, experimental reports focused on the observation of interlayer DMI, leaving the development of strategies to control interlayer DMI's magnitude unaddressed. Here, we introduce an azimuthal symmetry engineering protocol capable of additive/subtractive tuning of interlayer DMI through the control of wedge deposition of separate layers and demonstrate its capability to mediate field-free spin-orbit torque (SOT) magnetization switching in both orthogonally magnetized and synthetic antiferromagnetically coupled systems. Furthermore, we showcase that the spatial inhomogeneity brought about by wedge deposition can be suppressed by specific azimuthal engineering design, ideal for practical implementation. Our findings provide guidelines for effective manipulations of interlayer DMI strength, beneficial for the future design of SOT-MRAM or other spintronic devices utilizing interlayer DMI.

Recent advances in two-dimensional intrinsic ferromagnetic materials Fe3X(X=Ge and Ga)Te2 and their heterostructures for spintronics.

Owing to their atomic thicknesses, atomically flat surfaces, long-range spin textures and captivating physical properties, two-dimensional (2D) magnetic materials, along with their van der Waals heterostructures (vdWHs), have attracted much interest for the development of next-generation spin-based materials and devices. As an emergent family of intrinsic ferromagnetic materials, Fe3X(X=Ge and Ga)Te2 has become a rising star in the fields of condensed matter physics and materials science owing to their high Curie temperature and large perpendicular magnetic anisotropy. Herein, we aim to comprehensively summarize the recent progress on 2D Fe3X(X=Ge and Ga)Te2 and their vdWHs and provide a panorama of their physical properties and underlying mechanisms. First, an overview of Fe3X(X=Ge and Ga)Te2 is presented in terms of crystalline and electronic structures, distinctive physical properties and preparation methods. Subsequently, the engineering of electronic and spintronic properties of Fe3X(X=Ge and Ga)Te2 by diverse means, including strain, gate voltage, substrate and patterning, is surveyed. Then, the latest advances in spintronic devices based on 2D Fe3X(X=Ge and Ga)Te2 vdWHs are discussed and elucidated in detail, including vdWH devices that exploit the exchange bias effect, magnetoresistance effect, spin-orbit torque effect, magnetic proximity effect and Dzyaloshinskii-Moriya interaction. Finally, the future outlook is given in terms of efficient large-scale fabrication, intriguing physics and important technological applications of 2D Fe3X(X=Ge and Ga)Te2 and their vdWHs. Overall, this study provides an overview to support further studies of emergent 2D Fe3X(X=Ge and Ga)Te2 materials and related vdWH devices for basic science and practical applications.

Tunable long-range spin transport in a van der Waals Fe3GeTe2/WSe2/Fe3GeTe2 spin valve.

The seamless integration of two-dimensional (2D) ferromagnetic materials with similar or dissimilar materials can widen the scope of low-power spintronics. In this regard, a vertical van der Waals (vdW) heterostructure of 2D ferromagnets with semiconducting transition metal dichalcogenides (TMDCs) forms magnetic junctions with exceptional stability and electrical control. Interestingly, 2D metallic Fe3GeTe2 (FGT) reveals above room temperature Curie temperatures and has large magneto anisotropy due to spin-orbit coupling. In addition, it also possesses topological states and a large Berry curvature. Herein, we designed the FGT/WSe2/FGT vdW heterostructure with a uniform and sharp interface so that FGT could maintain its inherent electronic properties. Also, the uniform thickness of the barrier provides a smooth flow of spins through the junctions as tunneling exponentially decays with an increasing barrier thickness. However, strong energy-dependent spin polarization is crucial for achieving optimum spin valve properties, such as large tunneling magnetoresistance (TMR) along with the manipulation of the magnitude and sign reversal. We have observed a shifting of high-energy localized minority spin states toward low-energy regions, which causes spin polarization fluctuation between -42.5% and 41% over a wide range of bias voltage. This leads to a negative TMR% of ∼-100% at 0.1 V Å-1 and also a large positive TMR% at 0.2 V Å-1 and -0.4 V Å-1. Besides, the system exhibits a highly tunable large anomalous Hall conductivity (AHC) of 626 S cm-1. Interestingly, such unprecedented electronic behaviour with large and switchable spin polarization, anomalous Hall conductivity and TMR can be incorporated into MTJ devices, which provide electrical control and long-range spin transport. Additionally, the system emerges as a standout candidate in low-power spintronic devices (e.g., MRAM and magnetic sensors) owing to its distinctive energy-dependent electronic structure with a wide range of external bias.

Emergent self-duality in a long-range critical spin chain: From deconfined criticality to first-order transition

Emergent self-duality in a long-range critical spin chain: From deconfined criticality to first-order transition

Spin selectivity in elemental tellurium and other chiral materials

The phenomenon of chirality-induced spin selectivity (CISS), where chiral organic molecules enable the selective transmission of electrons spin-polarized along the direction of electric current, has been studied for nearly two decades. Despite its technological relevance, CISS is not fully understood. Recent studies have expanded the concept of spin selectivity to chiral inorganic crystals, offering promise for magnet-free spintronics and other applications. This Perspective reviews recent developments on spin selectivity in non-magnetic solid-state materials, whereby chirality-dependent charge-to-spin conversion is responsible for transforming electric currents into spin signals, and spin transport within devices. Notably, chiral systems often outperform non-chiral ones in terms of conversion efficiency and facilitate long-range spin transport, which makes them relevant for both fundamental and applied physics. After examining the archetypal example of the chiral crystal, elemental tellurium, and the studies of spin selectivity in Weyl semimetals, we discuss its origin in terms of the unconventional (collinear) Rashba–Edelstein effect. We also explore key factors affecting the conversion efficiency and robustness of spin transport, focusing on persistent spin textures and their influence on spin lifetime. In addition, we discuss the potential impact of band velocities and the role of orbital contributions, as well as the differences associated with reduced dimensionality, providing a roadmap for guiding future theoretical, experimental, and applied studies.

Continuously varying critical exponents in long-range quantum spin ladders

We investigate the quantum-critical behavior between the rung-singlet phase with hidden string order and the Néel phase with broken SU(2)-symmetry in quantum spin ladders with algebraically decaying unfrustrated long-range Heisenberg interactions. To this end, we determine high-order series expansions of energies and observables in the thermodynamic limit about the isolated rung-dimer limit. This is achieved by extending the method of perturbative continuous unitary transformations (pCUT) to long-range Heisenberg interactions and to the calculation of generic observables. The quantum-critical breakdown of the rung-singlet phase then allows us to determine the critical phase transition line and the entire set of critical exponents as a function of the decay exponent of the long-range interaction. We demonstrate long-range mean-field behavior as well as a non-trivial regime of continuously varying critical exponents implying the absence of deconfined criticality contrary to a recent suggestion in the literature.

One-Dimensional Van Der Waals Helical Crystals with an Irrational Twist

Long-range helicity in condensed materials has sternly relied on the precise ordering of cooperative intra- and inter-molecular bonding interactions. The exclusivity of these interactions in natural, organic, or molecular systems has limited the conclusive demonstration of aperiodic helical motifs in densely packed solid state lattices. In this talk, we will present a class of 1D van der Waals solids that crystallize as weakly bound helical chains that possess atomic scale order consistent with an aperiodic tetrahelix. We will describe how precise atomic level control of the local coordination environment in these 1D vdW lattices induces helical aperiodicity in periodic helical motifs based on repeating screw axis symmetry motifs. We will also highlight herein that the modularity of vdW lattices allows for the systematic engineering of helical attributes (radius, rise, and twist angle) and band gap energies across the visible to the near-UV spectral window. Owing to the intrinsic non-centrosymmetry of aperiodic helices, we will show that these 1D vdW tetrahelices exhibit visible range second harmonic generation in freestanding crystals from the bulk down to the nanoscale. Lastly, we will demonstrate that the weak vdW interchain interactions in these 1D vdW tetrahelices enables the micromechanical exfoliation into single ~1 nm diameter chiral helical chains. The realization of exfoliable 1D vdW tetrahelices presents a unique materials platform towards understanding the synthetic design rules towards helicity and chirality in low-dimensional solids. Atomically-precise helicity along these length scales will facilitate new opportunities in designing solid state materials towards sub-nanoscale nonlinear chiroptics, long-range spin polarization via chiral-induced spin selectivity, and 1D topological helicoid quantum states.

Giant spin Hall effect in AB-stacked MoTe2/WSe2 bilayers.

The spin Hall effect (SHE), in which an electrical current generates a transverse spin current, plays an important role in spintronics for the generation and manipulation of spin-polarized electrons. The phenomenon originates from spin-orbit coupling. In general, stronger spin-orbit coupling favours larger SHEs but shorter spin relaxation times and diffusion lengths. However, correlated magnetic materials often do not support large SHEs. Achieving large SHEs, long-range spin transport and magnetism simultaneously in a single material is attractive for spintronics applications but has remained a challenge. Here we demonstrate a giant intrinsic SHE coexisting with ferromagnetism in AB-stacked MoTe2/WSe2 moiré bilayers by direct magneto-optical imaging. Under moderate electrical currents with density <1 A m-1, we observe spin accumulation on transverse sample edges that nearly saturates the spin density. We also demonstrate long-range spin Hall transport and efficient non-local spin accumulation that is limited only by the device size (about 10 µm). The gate dependence shows that the giant SHE occurs only near the interaction-driven Chern insulating state. At low temperatures, it emerges after the quantum anomalous Hall breakdown. Our results demonstrate moiré engineering of Berry curvature and electronic correlation for potential spintronics applications.