Nonvolatile Electric Control of Antiferromagnet CrSBr.

van der Waals magnets are emerging as a promising material platform for electric field control of magnetism, offering a pathway toward the elimination of external magnetic fields from spintronic devices. A further step is the integration of such magnets with electrical gating components that would enable nonvolatile control of magnetic states. However, this approach remains unexplored for antiferromagnets, despite their growing significance in spintronics. Here, we demonstrate nonvolatile electric field control of magnetoelectric characteristics in van der Waals antiferromagnet CrSBr. We integrate a CrSBr channel in a flash-memory architecture featuring charge trapping graphene multilayers. The electrical gate operation triggers a nonvolatile 200% change in the antiferromagnetic state of CrSBr resistance by manipulating electron accumulation/depletion. Moreover, the nonvolatile gate modulates the metamagnetic transition field of CrSBr and the magnitude of magnetoresistance. Our findings highlight the potential of manipulating magnetic properties of antiferromagnetic semiconductors in a nonvolatile way.

Local control of superconductivity in a NbSe2/CrSBr van der Waals heterostructure.

Two-dimensional magnets and superconductors are emerging as tunable building-blocks for quantum computing and superconducting spintronic devices, and have been used to fabricate all two-dimensional versions of traditional devices, such as Josephson junctions. However, novel devices enabled by unique features of two-dimensional materials have not yet been demonstrated. Here, we present NbSe2/CrSBr van der Waals superconducting spin valves that exhibit infinite magnetoresistance and nonreciprocal charge transport. These responses arise from a unique metamagnetic transition in CrSBr, which controls the presence of localized stray fields suitably oriented to suppress the NbSe2 superconductivity in nanoscale regions and to break time reversal symmetry. Moreover, by integrating different CrSBr crystals in a lateral heterostructure, we demonstrate a superconductive spin valve characterized by multiple stable resistance states. Our results show how the unique physical properties of layered materials enable the realization of high-performance quantum devices based on novel working principles.

Defect-gradient-induced Rashba effect in van der Waals PtSe2 layers.

Defect engineering is one of the key technologies in materials science, enriching the modern semiconductor industry and providing good test-beds for solid-state physics. While homogenous doping prevails in conventional defect engineering, various artificial defect distributions have been predicted to induce desired physical properties in host materials, especially associated with symmetry breakings. Here, we show layer-by-layer defect-gradients in two-dimensional PtSe2 films developed by selective plasma treatments, which break spatial inversion symmetry and give rise to the Rashba effect. Scanning transmission electron microscopy analyses reveal that Se vacancies extend down to 7 nm from the surface and Se/Pt ratio exhibits linear variation along the layers. The Rashba effect induced by broken inversion symmetry is demonstrated through the observations of nonreciprocal transport behaviors and first-principles density functional theory calculations. Our methodology paves the way for functional defect engineering that entangles spin and momentum of itinerant electrons for emerging electronic applications.

Exchange Bias in Molecule/Fe3 GeTe2 van der Waals Heterostructures via Spinterface Effects.

The exfoliation of layered magnetic materials generates atomically thin flakes characterized by an ultrahigh surface sensitivity, which makes their magnetic properties tunable via external stimuli, such as electrostatic gating and proximity effects. Another powerful approach to engineer magnetic materials is molecular functionalization, generating hybrid interfaces with tailored magnetic interactions, called spinterfaces. However, spinterface effects have not yet been explored on layered magnetic materials. Here, the emergence of spinterface effects is demonstrated at the interface between flakes of the prototypical layered magnetic metal Fe3 GeTe2 and thin films of Co-phthalocyanine. Magnetotransport measurements show that the molecular layer induces a magnetic exchange bias in Fe3 GeTe2 , indicating that the unpaired spins in Co-phthalocyanine develop antiferromagnetic ordering and pin the magnetization reversal of Fe3 GeTe2 via magnetic proximity. The effect is strongest for a Fe3 GeTe2 thickness of 20 nm, for which the exchange bias field reaches -840 Oe at 10 K and is measurable up to ≈110 K. This value compares very favorably with previous exchange bias fields reported for Fe3 GeTe2 in all-inorganic van der Waals heterostructures, demonstrating the potential of molecular functionalization to tailor the magnetism of van der Waals layered materials.

A scalable molecule-based magnetic thin film for spin-thermoelectric energy conversion.

Spin thermoelectrics, an emerging thermoelectric technology, offers energy harvesting from waste heat with potential advantages of scalability and energy conversion efficiency, thanks to orthogonal paths for heat and charge flow. However, magnetic insulators previously used for spin thermoelectrics pose challenges for scale-up due to high temperature processing and difficulty in large-area deposition. Here, we introduce a molecule-based magnetic film for spin thermoelectric applications because it entails versatile synthetic routes in addition to weak spin-lattice interaction and low thermal conductivity. Thin films of CrII[CrIII(CN)6], Prussian blue analogue, electrochemically deposited on Cr electrodes at room temperature show effective spin thermoelectricity. Moreover, the ferromagnetic resonance studies exhibit an extremely low Gilbert damping constant ~(2.4 ± 0.67) × 10-4, indicating low loss of heat-generated magnons. The demonstrated STE applications of a new class of magnet will pave the way for versatile recycling of ubiquitous waste heat.

Observation of spin-polarized Anderson state around charge neutral point in graphene with Fe-clusters.

The pristine graphene described with massless Dirac fermion could bear topological insulator state and ferromagnetism via the band structure engineering with various adatoms and proximity effects from heterostructures. In particular, topological Anderson insulator state was theoretically predicted in tight-binding honeycomb lattice with Anderson disorder term. Here, we introduced physi-absorbed Fe-clusters/adatoms on graphene to impose exchange interaction and random lattice disorder, and we observed Anderson insulator state accompanying with Kondo effect and field-induced conducting state upon applying the magnetic field at around a charge neutral point. Furthermore, the emergence of the double peak of resistivity at ν = 0 state indicates spin-splitted edge state with high effective exchange field (>70 T). These phenomena suggest the appearance of topological Anderson insulator state triggered by the induced exchange field and disorder.

Gate-tunable giant nonreciprocal charge transport in noncentrosymmetric oxide interfaces.

A polar conductor, where inversion symmetry is broken, may exhibit directional propagation of itinerant electrons, i.e., the rightward and leftward currents differ from each other, when time-reversal symmetry is also broken. This potential rectification effect was shown to be very weak due to the fact that the kinetic energy is much higher than the energies associated with symmetry breaking, producing weak perturbations. Here we demonstrate the appearance of giant nonreciprocal charge transport in the conductive oxide interface, LaAlO3/SrTiO3, where the electrons are confined to two-dimensions with low Fermi energy. In addition, the Rashba spin-orbit interaction correlated with the sub-band hierarchy of this system enables a strongly tunable nonreciprocal response by applying a gate voltage. The observed behavior of directional response in LaAlO3/SrTiO3 is associated with comparable energy scales among kinetic energy, spin-orbit interaction, and magnetic field, which inspires a promising route to enhance nonreciprocal response and its functionalities in spin orbitronics.

Molecular Tunability of Magnetic Exchange Bias and Asymmetrical Magnetotransport in Metalloporphyrin/Co Hybrid Bilayers.

Individual molecular spins are promising quantum states for emerging computation technologies. The "on surface" configuration of molecules in proximity to a magnetic film allows control over the orientations of molecular spins and coupling between them. The stacking of planar molecular spins could favor antiferromagnetic interlayer couplings and lead to pinning of the magnetic underlayer via the exchange bias, which is extensively utilized in ultrafast and high-density spintronics. However, fundamental understanding of the molecular exchange bias and its operating features on a device has not been unveiled. Here, we showed tunable molecular exchange bias and its asymmetrical magnetotransport characteristics on a device by using the metalloporphyrin/cobalt hybrid films. A series of the distinctive molecular layers showcased a wide range of the interfacial exchange coupling and bias. The transport behaviors of the hybrid bilayer films revealed the molecular exchange bias effect on a fabricated device, representing asymmetric characteristics on anisotropic and angle-dependent magnetoresistances. Theoretical simulations demonstrated close correlations among the interfacial distance, magnetic interaction, and exchange bias. This study of the hybrid interfacial coupling and its impact on magnetic and magnetotransport behaviors will extend functionalities of molecular spinterfaces for emerging information technologies.

Solution-Processed Ferrimagnetic Insulator Thin Film for the Microelectronic Spin Seebeck Energy Conversion.

The longitudinal spin Seebeck effects with a ferro- or ferrimagnetic insulator provide a new architecture of a thermoelectric device that could significantly improve the energy conversion efficiency. Until now, epitaxial yttrium iron garnet (YIG) films grown on gadolinium gallium garnet (GGG) substrates by a pulsed laser deposition have been most widely used for spin thermoelectric energy conversion studies. In this work, we developed a simple route to obtain a highly uniform solution-processed YIG film and used it for the on-chip microelectronic spin Seebeck characterization. We improved the film roughness down to ∼0.2 nm because the extraction of thermally induced spin voltage relies on the interfacial quality. The on-chip microelectronic device has a dimension of 200 µm long and 20 µm wide. The solution-processed 20 nm thick YIG film with a 10 nm Pt film was used for the spin Seebeck energy converter. For a temperature difference of Δ T ≈ 0.036 K applied on the thin YIG film, the obtained Δ V ≈ 28 µV, which is equivalent to SLSSE ≈ 80.4 nV/K, is close to the typical reported values for thick epitaxial YIG films. The temperature and magnetic field-dependent behaviors of spin Seebeck effects in our YIG films suggest active magnon excitations through the noncoherent precession channel. The effective SSE generation with the solution-processed thin YIG film provides versatile applications of the spin thermoelectric energy conversion.

Atomic Scale Study on Growth and Heteroepitaxy of ZnO Monolayer on Graphene.

Atomically thin semiconducting oxide on graphene carries a unique combination of wide band gap, high charge carrier mobility, and optical transparency, which can be widely applied for optoelectronics. However, study on the epitaxial formation and properties of oxide monolayer on graphene remains unexplored due to hydrophobic graphene surface and limits of conventional bulk deposition technique. Here, we report atomic scale study of heteroepitaxial growth and relationship of a single-atom-thick ZnO layer on graphene using atomic layer deposition. We demonstrate atom-by-atom growth of zinc and oxygen at the preferential zigzag edge of a ZnO monolayer on graphene through in situ observation. We experimentally determine that the thinnest ZnO monolayer has a wide band gap (up to 4.0 eV), due to quantum confinement and graphene-like structure, and high optical transparency. This study can lead to a new class of atomically thin two-dimensional heterostructures of semiconducting oxides formed by highly controlled epitaxial growth.

Nonlocal Spin Diffusion Driven by Giant Spin Hall Effect at Oxide Heterointerfaces.

A two-dimensional electron gas emerged at a LaAlO3/SrTiO3 interface is an ideal system for "spin-orbitronics" as the structure itself strongly couple the spin and orbital degree of freedom through the Rashba spin-orbit interaction. One of core experiments toward this direction is the nonlocal spin transport measurement, which has remained elusive due to the low spin injection efficiency to this system. Here we bypass the problem by generating a spin current not through the spin injection from outside but instead through the inherent spin Hall effect and demonstrate the nonlocal spin transport. The analysis on the nonlocal spin voltage, confirmed by the signature of a Larmor spin precession and its length dependence, displays that both D'yakonov-Perel' and Elliott-Yafet mechanisms involve in the spin relaxation at low temperature. Our results show that the oxide heterointerface is highly efficient in spin-charge conversion with exceptionally strong spin Hall coefficient γ ∼ 0.15 ± 0.05 and could be an outstanding platform for the study of coupled charge and spin transport phenomena and their electronic applications.

Gate-Tunable Spin Exchange Interactions and Inversion of Magnetoresistance in Single Ferromagnetic ZnO Nanowires.

Electrical control of ferromagnetism in semiconductor nanostructures offers the promise of nonvolatile functionality in future semiconductor spintronics. Here, we demonstrate a dramatic gate-induced change of ferromagnetism in ZnO nanowire (NW) field-effect transistors (FETs). Ferromagnetism in our ZnO NWs arose from oxygen vacancies, which constitute deep levels hosting unpaired electron spins. The magnetic transition temperature of the studied ZnO NWs was estimated to be well above room temperature. The in situ UV confocal photoluminescence (PL) study confirmed oxygen vacancy mediated ferromagnetism in the studied ZnO NW FET devices. Both the estimated carrier concentration and temperature-dependent conductivity reveal the studied ZnO NWs are at the crossover of the metal-insulator transition. In particular, gate-induced modulation of the carrier concentration in the ZnO NW FET significantly alters carrier-mediated exchange interactions, which causes even inversion of magnetoresistance (MR) from negative to positive values. Upon sweeping the gate bias from -40 to +50 V, the MRs estimated at 2 K and 2 T were changed from -11.3% to +4.1%. Detailed analysis on the gate-dependent MR behavior clearly showed enhanced spin splitting energy with increasing carrier concentration. Gate-voltage-dependent PL spectra of an individual NW device confirmed the localization of oxygen vacancy-induced spins, indicating that gate-tunable indirect exchange coupling between localized magnetic moments played an important role in the remarkable change of the MR.

Roles of plant hormones and anti-apoptosis genes during drought stress in rice (Oryza sativa L.).

We previously identified the rice (Oryza sativa) senescence-associated gene OsSAP which encodes a highly conserved protein involved in anti-apoptotic activity. This novel Bax suppressor-related gene regulates tolerance to multiple stresses in yeast. Here, we show the effects of drought stress on leaf and root tissues of plants over-expressing OsSAP in relation to the levels of phytohormones, abscisic acid (ABA), jasmonic acid (JA), indole-3-carboxylic acid (ICA), gibberellic acid (GA3), and zeatin. Results showed that rice plants over-expressing SAP were tolerant to drought stress compared to wild type and the plants over-expressing AtBI-1, which is a homolog of the human Bax inhibitor-1 in Arabidopsis. ABA and JA levels in OsSAP and AtBI-1 transgenic plants consistently increased up to at least 3 days after drought treatment, whereas lower GA3 levels were recorded during early drought period. Comparison between control and transgenic plants overexpressing anti-apoptosis genes OsSAP and AtBI-1 resulted in different patterns of hormone levels, indicating that these genes are involved in the plant responses to drought stress and present an opportunity for further study on drought stress tolerance in rice and other plant species.

Effects of TiO2 interfacial atomic layers on device performances and exciton dynamics in ZnO nanorod polymer solar cells.

The performances of organic electronic and/or photonic devices rely heavily on the nature of the inorganic/organic interface. Control over such hybrid interface properties has been an important issue for optimizing the performances of polymer solar cells bearing metal-oxide conducting channels. In this work, we studied the effects of an interfacial atomic layer in an inverted polymer solar cell based on a ZnO nanorod array on the device performance as well as the dynamics of the photoexcited carriers. We adopted highly conformal TiO2 interfacial layer using plasma enhanced atomic layer deposition (PEALD) to improve the compatibility between the solution-prepared active layer and the ZnO nanorod array. The TiO2 interfacial layer facilitated exciton separation and subsequent charge transfer into the nanorod channel, and it suppressed recombination of photogenerated carriers at the interface. The presence of even 1 PEALD cycle of TiO2 coating substantially improved the short-circuit current density (Jsc), open circuit voltage (Voc), and fill factor (FF), leading to more than 2-fold enhancement in the power conversion efficiency (PCE). The dynamics of the photoexcited carriers in our devices were studied using transient absorption (TA) spectroscopy. The TA results clearly revealed that the TiO2 coating played a key role as an efficient quencher of photogenerated excitons, thereby reducing the exciton lifetime. The electrochemical impedance spectra (EIS) provided further evidence that the TiO2 atomic interfacial layer promoted the charge transfer at the interface by suppressing recombination loss.