Thermally Driven Spin Transport of Epitaxial FeRh Films with a Non-magnetic Pt Layer via the Longitudinal Spin Seebeck Effect.

FeRh has been demonstrated to be an important material for the observation of magnetic phase transitions, such as the first-order transition from an antiferromagnetic (AFM) to a ferromagnetic (FM) state, in response to changes in the temperature. This is because of the magnetic moment induced in Rh atoms above the magnetic phase transition temperature. In the present study, we focus on the longitudinal spin Seebeck effect (LSSE), which involves the generation of spin voltage as a result of a temperature gradient in FM materials or FM insulators, and experimentally assess the effect of the crystalline quality of FeRh films and the properties of the substrate on the LSSE thermopower during the FM-AFM phase transition. The measured LSSE thermopower of an epitaxial (110)-oriented FeRh film grown on an Al2O3 substrate is approximately 60 times higher than that of a polycrystalline FeRh film on a SiO2/Si substrate. This can be explained by the high magnetic sensitivity and superior FM properties of (110)-oriented epitaxial FeRh films. Furthermore, by comparing the transverse thermoelectric voltage for in-plane magnetized (IM) and perpendicularly magnetized (PM) configurations, we quantitively evaluate the contribution of the exclusive anomalous Nernst effect (ANE) to the LSSE signals in the FeRh/Al2O3 structure, finding it to be approximately 15-30% over a temperature range of 75-300 K. LSSE measurements in Pt/FeRh films are thus demonstrated to provide a versatile pathway for the development of thermoelectric power generation applications and other practical spintronics and neuromorphic computing devices.

Abnormal Magnetic Phase Transition in Mixed-Phase (110)-Oriented FeRh Films on Al2O3 Substrates via the Anomalous Nernst Effect.

Iron rhodium (FeRh) undergoes a first-order anti-ferromagnetic to ferromagnetic phase transition above its Curie temperature. By measuring the anomalous Nernst effect (ANE) in (110)-oriented FeRh films on Al2O3 substrates, the ANE thermopower over a temperature range of 100-350 K is observed, with similar magnetic transport behaviors observed for in-plane magnetization (IM) and out-of-plane magnetization (PM) configurations. The temperature-dependent magnetization-magnetic field strength (M-H) curves revealed that the ANE voltage is proportional to the magnetization of the material, but additional features magnetic textures not shown in the M-H curves remained intractable. In particular, a sign reversal occurred for the ANE thermopower signal near zero field in the mixed-magnetic-phase films at low temperatures, which is attributed to the diamagnetic properties of the Al2O3 substrate. Finite element method simulations associated with the Heisenberg spin model and Landau-Lifshitz-Gilbert equation strongly supported the abnormal heat transport behavior from the Al2O3 substrate during the experimentally observed magnetic phase transition for the IM and PM configurations. The results demonstrate that FeRh films on an Al2O3 substrate exhibit unusual behavior compared to other ferromagnetic materials, indicating their potential for use in novel applications associated with practical spintronics device design, neuromorphic computing, and magnetic memory.

Ab-initioprediction of gigantic anomalous Nernst effect in ferromagnetic monolayer transition metal trihalides.

The anomalous Hall conductivity of all transition metal trihalides was explored using first-principles calculations. Employing the Fukui-Hatsugai-Suzuki method, we found that ferromagnetic monolayersXBr3(X= Pd, Pt) possessed the quantized anomalous Hall conductivity (QAHC) with and without carrier doping. Due to unique QAHC, their transverse thermoelectric properties ofXBr3(X= Pd, Pt) were investigated. Employing the semi-classical Boltzmann transport theory, the transverse thermoelectric coefficient of each monolayer was analyzed. Anomalous Nernst coefficients (ANCs) of theXBr3monolayers were prominent both at and near the Fermi level. Under an assumed relaxation time of 10 fs, the maximum ANCs for the PdBr3(PtBr3) monolayer reached -54.1 (-23.3)µV K-1atT=300 K upon doping with 1.21 × 1014(5.64 × 1013) holes cm-2. The large ANCs of theXBr3monolayers were attributed to the opening of a narrow bandgap generated by spin-orbit coupling both at and near the Fermi level, which led to a large Seebeck-induced charge current and large anomalous Nernst conductivity. These results suggest that ferromagneticXBr3monolayers have significant potential for application in thermoelectric devices.

Spin caloritronics in metallic superlattices.

Spin caloritronics, a research field studying on the interconversion between a charge current (Jc) and a heat current (Jq) mediated by a spin current (Js) and/or magnetization (M), has attracted much attention not only for academic interest but also for practical applications. Newly discovered spin-caloritronic phenomena such as the spin Seebeck effect (SSE) have stimulated the renewed interest in the thermoelectric phenomena of a magnet, which have been known for a long time, e.g. the anomalous Nernst effect (ANE). These spin-caloritronic phenomena involving the SSE and the ANE have provided with a new direction for thermoelectric conversion exploitingJsand/orM. Importantly, the symmetry of ANE allows the thermoelectric conversion in the transverse configuration betweenJqandJc. Although the transverse configuration is totally different from the conventional longitudinal configuration based on the Seebeck effect and has many advantages, we are still facing several issues that need to be solved before developing practical applications. The primal issue is the improvement of conversion efficiency. In the case of ANE-based applications, a material with a large anomalous Nernst coefficient (SANE) is the key for solving the issue. This review article introduces the increase ofSANEcan be achieved by forming superlattice structures, which has been demonstrated for several kinds of materials combinations. The overall picture of studies on spin caloritronics is first surveyed. Then, we mention the pioneering work on the transverse thermoelectric conversion in superlattice structures, which was performed using Fe-based metallic superlattices, and show the recent studies for the Ni-based metallic superlattices and the ordered alloy-based metallic superlattices.

Direct-Contact Seebeck-Driven Transverse Magneto-Thermoelectric Generation in Magnetic/Thermoelectric Bilayers.

Transverse thermoelectric generation converts temperature gradient in one direction into an electric field perpendicular to that direction and is expected to be a promising alternative in creating simple-structured thermoelectric modules that can avoid the challenging problems facing traditional Seebeck-effect-based modules. Recently, large transverse thermopower has been observed in closed circuits consisting of magnetic and thermoelectric materials, called the Seebeck-driven transverse magneto-thermoelectric generation (STTG). However, the closed-circuit structure complicates its broad applications. Here, STTG is realized in the simplest way to combine magnetic and thermoelectric materials, namely, by stacking a magnetic layer and a thermoelectric layer together to form a bilayer. The transverse thermopower is predicted to vary with changing layer thicknesses and peaks at a much larger value under an optimal thickness ratio. This behavior is verified in the experiment, through a series of samples prepared by depositing Fe-Ga alloy thin films of various thicknesses onto n-type Si substrates. The measured transverse thermopower reaches 15.2 ± 0.4 µV K-1, which is a fivefold increase from that of Fe-Ga alloy and much larger than the current room temperature record observed in Weyl semimetal Co2MnGa. The findings highlight the potential of combining magnetic and thermoelectric materials for transverse thermoelectric applications.

Angular Position Sensor Based on Anisotropic Magnetoresistive and Anomalous Nernst Effect.

Magnetic position sensors have extensive applications in various industrial sectors and consumer products. However, measuring angles in the full range of 0-360° in a wide field range using a single magnetic sensor remains a challenge. Here, we propose a magnetic position sensor based on a single Wheatstone bridge structure made from a single ferromagnetic layer. By measuring the anisotropic magnetoresistance (AMR) signals from the bridge and two sets of anomalous Nernst effect (ANE) signals from the transverse ports on two perpendicular Wheatstone bridge arms concurrently, we show that it is possible to achieve 0-360° angle detection using a single bridge sensor. The combined use of AMR and ANE signals allows a mean angle error in the range of 0.51-1.05° within a field range of 100 Oe-10,000 Oe to be achieved.

Optical transparency in 2D ferromagnetic WSe2/1T-VSe2/WSe2multilayer with strain induced large anomalous Nernst conductivity.

Transparent two-dimensional (2D) magnetic materials may bring intriguing features and are indispensable for transparent electronics. However, it is rare to find both optical transparency and room-temperature ferromagnetism simultaneously in a single 2D material. Herein, we explore the possibility of both these features in 2D WSe2/1T-VSe2(1ML)/WSe2and WSe2/1T-VSe2(2ML)/WSe2heterostructures by taking one monolayer (1ML) and two monolayers (2ML) of 1T-VSe2using first-principles calculations. Further, we investigate anomalous Hall conductivity (AHC) and anomalous Nernst conductivity (ANC) using a maximally localized Wannier function. The WSe2/1T-VSe2(1ML)/WSe2and WSe2/1T-VSe2(2ML)/WSe2systems show Curie temperatures of 328 and 405 K. Under biaxial compressive strain, the magnetic anisotropy of both systems is switched from in-plane to out-of-plane. We find a large AHC of 1.51 e2/h and 3.10 e2/h in the electron-doped region for strained WSe2/1T-VSe2(1ML)/WSe2and WSe2/1T-VSe2(2ML)/WSe2systems. Furthermore, we obtain a giant ANC of 3.94 AK-1m-1in a hole-doped strained WSe2/1T-VSe2(2ML)/WSe2system at 100 K. Both WSe2/1T-VSe2(1ML)/WSe2and WSe2/1T-VSe2(2ML)/WSe2are optically transparent in the visible ranges with large refractive indices of 3.2-3.4. Our results may suggest that the WSe2/1T-VSe2/WSe2structure possesses multifunctional physical properties and these features can be utilized for spintronics and optoelectronics device applications such as magnetic sensors, memory devices, and transparent magneto-optic devices at room temperature.

Efficient Thermo-Spin Conversion in van der Waals Ferromagnet FeGaTe.

Recent discovery of 2D van der Waals magnetic materials has spurred progress in developing advanced spintronic devices. A central challenge lies in enhancing the spin-conversion efficiency for building spin-logic or spin-memory devices. Here, the anomalous Hall and Nernst effects are systematically investigated to uncover significant spin-conversion effects in above-room-temperature van der Waals ferromagnet FeGaTe with perpendicular magnetic anisotropy. The anomalous Hall effect demonstrates an efficient electric spin-charge conversion with a notable spin Hall angle of over 6%. In addition, the anomalous Nernst effect produces a significant transverse voltage at room temperature without a magnetic field, displaying unique temperature dependence with a maximum transverse Seebeck coefficient of 440 nV K-1 and a Nernst angle of ≈62%. Such an innovative thermoelectric signal arises from the efficient thermo-spin conversion effect, where the up-spin and down-spin electrons move in opposite directions under a temperature gradient. The present study highlights the potential of FeGaTe to enhance thermoelectric devices through efficient thermo-spin conversion without the need for a magnetic field.

Large Thermo-Spin Effects in Heusler Alloy-Based Spin Gapless Semiconductor Thin Films.

Recently, Heusler alloy-based spin gapless semiconductors (SGSs) with high Curie temperature (TC) and sizable spin polarization have emerged as potential candidates for tunable spintronic applications. We report comprehensive investigation of the temperature-dependent ANE and intrinsic longitudinal spin Seebeck effect (LSSE) in CoFeCrGa thin films grown on MgO substrates. Our findings show that the anomalous Nernst coefficient for the MgO/CoFeCrGa (95 nm) film is ≈1.86 µV K-1 at room temperature, which is nearly 2 orders of magnitude higher than that of the bulk polycrystalline sample of CoFeCrGa (≈0.018 µV K-1) and almost 3 orders of magnitude higher than that of the half-metallic ferromagnet La1-xNaxMnO3 (≈0.005 µV K-1) but comparable to that of the magnetic Weyl semimetal Co2MnGa thin film (≈2-3 µV K-1). Furthermore, the LSSE coefficient for our MgO/CoFeCrGa (95 nm)/Pt (5 nm) heterostructure is ≈20.5 nV K-1 Ω-1 at room temperature, which is twice larger than that of the half-metallic ferromagnetic La0.7Sr0.3MnO3 thin films (≈9 nV K-1 Ω-1). We show that both ANE and LSSE coefficients follow identical temperature dependences and exhibit a maximum at ≈225 K, which is understood as the combined effects of inelastic magnon scatterings and reduced magnon population at low temperatures. Our analyses not only indicate that the extrinsic skew scattering is the dominating mechanism for ANE in these films but also provide critical insights into the functional form of the observed temperature-dependent LSSE at low temperatures. Furthermore, by employing radio frequency transverse susceptibility and broad-band ferromagnetic resonance in combination with the LSSE measurements, we establish a correlation among the observed LSSE signal, magnetic anisotropy, and Gilbert damping of the CoFeCrGa thin films, which will be beneficial for fabricating tunable and highly efficient Heusler alloy-based spin caloritronic nanodevices.

Giant, Linearly Increasing Spin-Orbit Torque Efficiency in Symmetry-Broken Spin-Orbit Torque Superlattices.

Magnetic heterostructures with high spin-orbit torque efficiency and low impedance have great promise for low-power spintronic technologies. We report a symmetry-broken spin-orbit superlattice [Pt0.75Cu0.25/Co/Ta]n, in which the dampinglike spin-orbit torque efficiency accumulates linearly with the repeat number n and achieves a giant value of >200% when n = 16, which is 100 times stronger than that of a conventional magnetic heterostructure with a clean Pt (e.g., 2% at a resistivity of 7 µΩ cm). The giant spin-orbit torque effect arises predominantly from the spin Hall effect of Pt0.75Cu0.25. The anomalous Nernst effect increases remarkably as the repeat number n increases, implying a critical need to include the thermal effect in the analysis of magnetic superlattices and multilayers. The giant spin-orbit torque, low resistivity, and strong anomalous Nernst effect suggest the great potential of the superlattice [Pt0.75Cu0.25/Co/Ta]n for low-power memory and logic technologies as well as high-performance thermoelectric battery and sensor applications.

Longitudinal Spin Seebeck Effect Thermopiles Based on Flexible Co-Rich Amorphous Ribbons/Pt Thin-Film Heterostructures.

Thermoelectric phenomena, such as the Anomalous Nernst and Longitudinal Spin Seebeck Effects, are promising for sensor applications in the area of renewable energy. In the case of flexible electronic materials, the request is even larger because they can be integrated into devices having complex shape surfaces. Here, we reveal that Pt promotes an enhancement of the thermoelectric response in Co-rich ribbon/Pt heterostructures due to the spin-to-charge conversion. Moreover, we demonstrated that the employment of the thermopiles configuration in this system increases the induced thermoelectric current, a fact related to the considerable decrease in the electric resistance of the system. By comparing present findings with the literature, we were able to design a flexible thermopile based on LSSE without the lithography process. Additionally, the thermoelectric voltage found in the studied flexible heterostructures is comparable to the ones verified for rigid systems.

Anomalous Nernst Effect Induced Terahertz Emission in a Single Ferromagnetic Film.

Despite its important role in understanding ultrafast spin dynamics and revealing novel spin/orbit effects, the mechanism of the terahertz (THz) emission from a single ferromagnetic nanofilm upon a femtosecond laser pump still remains elusive. Recent experiments have shown exotic symmetry, which is not expected from the routinely adopted mechanism of ultrafast demagnetization. Here, by developing a bidirectional pump-THz emission spectroscopy and associated symmetry analysis method, we set a benchmark for the experimental distinction of the THz emission induced by various mechanisms. Our results unambiguously unveil a new mechanism─anomalous Nernst effect (ANE) induced THz emission due to the ultrafast temperature gradient created by a femtosecond laser. Quantitative analysis shows that the THz emission exhibits interesting thickness dependence where different mechanisms dominate at different thickness ranges. Our work not only clarifies the origin of the ferromagnetic-based THz emission but also offers a fertile platform for investigating the ultrafast optomagnetism and THz spintronics.

Large Anomalous Nernst Effects at Room Temperature in Fe3 Pt Thin Films.

Heat current in ferromagnets can generate a transverse electric voltage perpendicular to magnetization, known as anomalous Nernst effect (ANE). ANE originates intrinsically from the combination of large Berry curvature and density of states near the Fermi energy. It shows technical advantages over the conventional longitudinal Seebeck effect in converting waste heat to electricity due to its unique transverse geometry. However, materials showing giant ANE remain to be explored. Herein,  a large ANE thermopower of Syx ≈ 2 µV K-1 at room temperature in ferromagnetic Fe3 Pt epitaxial films is reported, which also show a giant transverse thermoelectric conductivity of αyx ≈ 4 A K-1  m-1 and a remarkable coercive field of 1300 Oe. The theoretical analysis reveals that the strong spin-orbit interaction in addition to the hybridization between Pt 5d and Fe 3d electrons leads to a series of distinct energy gaps and large Berry curvature in the Brillouin zone, which is the key for the large ANE. These results highlight the important roles of both Berry curvature and spin-orbit coupling in achieving large ANE at zero magnetic field, providing pathways to explore materials with giant transverse thermoelectric effect without an external magnetic field.

Tuning the anomalous Nernst and Hall effects with shifting the chemical potential in Fe-doped and Ni-doped Co3Sn2S2.

Co3Sn2S2is believed to be a magnetic Weyl semimetal. It displays large anomalous Hall, Nernst and thermal Hall effects with a remarkably large anomalous Hall angle. Here, we present a comprehensive study of how substituting Co by Fe or Ni affects the electrical and thermoelectric transport. We find that doping alters the amplitude of the anomalous transverse coefficients. The maximum decrease in the amplitude of the low-temperature anomalous Hall conductivityσijAis twofold. Comparing our results with theoretical calculations of the Berry spectrum assuming a rigid shift of the Fermi level, we find that given the modest shift in the position of the chemical potential induced by doping, the experimentally observed variation occurs five times faster than expected. Doping affects the amplitude and the sign of the anomalous Nernst coefficient. Despite these drastic changes, the amplitude of theαijA/σijAratio at the Curie temperature remains close to≈0.5kB/e, in agreement with the scaling relationship observed across many topological magnets.

Roll-to-Roll Printing of Anomalous Nernst Thermopile for Direct Sensing of Perpendicular Heat Flux.

The anomalous Nernst effect (ANE) converts heat flux perpendicular to the plane into electricity, in sharp contrast with the Seebeck effect (SE), enabling mass production, large area, and flexibility of their devices through ordinary thin-film fabrication techniques. Heat flux sensors, one of the most promising applications of ANE, are powerful devices for evaluating heat flow and can lead to energy savings through efficient thermal management. In reality, however, SE caused by the in-plane heat flux is always superimposed on the measurement signal, making it difficult to evaluate the perpendicular heat flux. Here, ANE-type heat flux sensors that selectively detect a perpendicular heat flux are fabricated by adjusting the net Seebeck coefficient in their thermopile circuit with mass-producible roll-to-roll sputtering methods. The direct sensing of perpendicular heat flux using ANE-based flexible thermopiles, as well as their simple fabrication process, paves the way for the practical application of thin-film thermoelectric devices.

Anomalous Nernst Effect in Flexible Co-Based Amorphous Ribbons.

Fe3Co67Cr3Si15B12 ribbons with a high degree of flexibility and excellent corrosion stability were produced by rapid quenching technique. Their structural, magnetic, and thermomagnetic (Anomalous Nernst Effect) properties were studied both in an as-quenched (NR) state and after stress annealing during 1 h at the temperature of 350 °C and a specific load of 230 MPa (AR). X-ray diffraction was used to verify the structural characteristics of our ribbons. Static magnetic properties were explored by inductive technique and vibrating sample magnetometry. The thermomagnetic curves investigated through the Anomalous Nernst Effect are consistent with the obtained magnetization results, presenting a linear response in the thermomagnetic signal, an interesting feature for sensor applications. Additionally, Anomalous Nernst Effect coefficient SANE values of 2.66µV/K and 1.93µV/K were estimated for the as-quenched and annealed ribbons, respectively. The interplay of the low magnetostrictive properties, soft magnetic behavior, linearity of the thermomagnetic response, and flexibility of these ribbons place them as promising systems to probe curved surfaces and propose multifunctional devices, including magnetic field-specialized sensors.

Proximity induced longitudinal and transverse thermoelectric response in graphene-ferromagnetic CrBr3vdW heterostructure.

The integration of longitudinal and transverse thermoelectric (TE) fosters various new opportunities in tuning the charge transport behaviour and opens a platform for efficient thermopower devices. The presence of asymmetric electronic structure supposed to accomplish large thermopower and electronic figure of merit. Herein, we investigate magnetic proximity coupled longitudinal and transverse TE behaviour in heterostructure of monolayer semimetal, graphene and a monolayer ferromagnet, CrBr3under the framework ofab initio-based calculations and employed constant relaxation time approximation (CRTA).The integrated density of states is elevated and asymmetric near Fermi energy region due to seamless proximity integration, depicting mixed character of graphene and CrBr3. The asymmetric nature of electronic structure significantly affects the Seebeck coefficients (S) and electrical conductivity (σ/τ) of heterostructure. The consistent step-like conductance spectrum influences interfacial polarization due to agile proximity integration. The magnitude of Seebeck coefficient (S) is found to be 653µV K-1near Fermi level. The heterostructure observes higher electrical conductivity and power factor in n-type region of the order of 106S m-1and 1020cm-3at room temperature. The dimensionless electronic figure of merit (zTe) advocates the heterostructure system to be an ideal TE material. Alongside longitudinal TE, we also find the heterostructure system is sensitive to anomalous Nernst effect (ANE) (transverse TE) with oscillatory nature. The Seebeck and ANE shows high degree of tunability with applied external electric field. The synergistic existence of Seebeck and ANE due to proximity integration in van der Waals atomic crystal at room temperature will provide realistic approach to experimentally fabricate and develop real-time thermopower devices.

Spin Seebeck Effect in Iron Oxide Thin Films: Effects of Phase Transition, Phase Coexistence, And Surface Magnetism.

Understanding the effects of phase transition, phase coexistence, and surface magnetism on the longitudinal spin Seebeck effect (LSSE) in a magnetic system is essential to manipulate the spin to charge current conversion efficiency for spincaloritronic applications. We aim to elucidate these effects by performing a comprehensive study of the temperature dependence of the LSSE in biphase iron oxide (BPIO = α-Fe2O3 + Fe3O4) thin films grown on Si (100) and Al2O3 (111) substrates. A combination of a temperature-dependent anomalous Nernst effect (ANE) and electrical resistivity measurements show that the contribution of the ANE from the BPIO layer is negligible in comparison to the intrinsic LSSE in the Si/BPIO/Pt heterostructure, even at room temperature. Below the Verwey transition of the Fe3O4 phase, the total signal across BPIO/Pt is dominated by the LSSE. Noticeable changes in the intrinsic LSSE signal for both Si/BPIO/Pt and Al2O3/BPIO/Pt heterostructures around the Verwey transition of the Fe3O4 phase and the antiferromagnetic (AFM) Morin transition of the α-Fe2O3 phase are observed. The LSSE signal for Si/BPIO/Pt is found to be almost 2 times greater than that for Al2O3/BPIO/Pt; however, an opposite trend is observed for the saturation magnetization. Magnetic force microscopy reveals the higher density of surface magnetic moments of the Si/BPIO film in comparison to the Al2O3/BPIO film, which underscores the dominant role of interfacial magnetism on the LSSE signal and thereby explains the larger LSSE for Si/BPIO/Pt.

Large magnon-induced anomalous Nernst conductivity in single-crystal MnBi.

Thermoelectric modules are a promising approach to energy harvesting and efficient cooling. In addition to the longitudinal Seebeck effect, transverse devices utilizing the anomalous Nernst effect (ANE) have recently attracted interest. For high conversion efficiency, it is required that the material have a large ANE thermoelectric power and low electrical resistance, which lead to the conductivity of the ANE. ANE is usually explained in terms of intrinsic contributions from Berry curvature. Our observations suggest that extrinsic contributions also matter. Studying single-crystal manganese-bismuth (MnBi), we find a high ANE thermopower (∼10 µV/K) under 0.6 T at 80 K, and a transverse thermoelectric conductivity of over 40 A/Km. With insight from theoretical calculations, we attribute this large ANE predominantly to a new advective magnon contribution arising from magnon-electron spin-angular momentum transfer. We propose that introducing a large spin-orbit coupling into ferromagnetic materials may enhance the ANE through the extrinsic contribution of magnons.

A Monomaterial Nernst Thermopile with Hermaphroditic Legs.

A large transverse thermoelectric response, known as the anomalous Nernst effect (ANE) has been recently observed in several topological magnets. Building a thermopile employing this effect has been the subject of several recent propositions. Here, a thermopile is designed and built with an array of tilted adjacent crystals of Mn3 Sn. The design employs a single material and replaces pairs of P and N thermocouples of the traditional design with hermaphroditic legs. The design exploits the large lag angle between the applied field and the magnetization, which is attributed to the interruption of magnetic octupoles at the edge of the xy-plane. Eliminating extrinsic contact between the legs will boost the efficiency, simplify the process, and pave the way for a new generation of thermopiles.