Experimental observation of current-driven antiskyrmion sliding in stripe domains.

Magnetic skyrmions are promising as next-generation information units. Their antiparticle-the antiskyrmion-has also been discovered in chiral magnets. Here we experimentally demonstrate antiskyrmion sliding in response to a pulsed electric current at room temperature without the requirement of an external magnetic field. This is realized by embedding antiskyrmions in helical stripe domains, which naturally provide one-dimensional straight tracks along which antiskyrmion sliding can be easily launched with low current density and without transverse deflection from the antiskyrmion Hall effect. The higher mobility of the antiskyrmions in the background of helical stripes in contrast to the typical ferromagnetic state is a result of intrinsic material parameters and elastic energy of the stripe domain, thereby smearing out the random pinning potential, as supported by micromagnetic simulations. The demonstration and comprehensive understanding of antiskyrmion movement along naturally straight tracks offers a new perspective for (anti)skyrmion application in spintronics.

Spontaneous Biskyrmion Lattice in a Centrosymmetric Rhombohedral Rare-Earth Magnet with Easy-Plane Anisotropy.

Magnetic skyrmion and its derivatives have demonstrated fascinating topological behaviors with potential applications in future spintronic devices. Despite the recent progress, the spontaneous skyrmion lattice and successive topological transition in the magnets with easy-plane magnetic anisotropy are still elusive especially at room temperature. Here, in a centrosymmetric rhombohedral Nd2Co17 magnet with easy-plane magnetic anisotropy, spontaneous biskyrmions are observed over a wide temperature range across room temperature, and then evolve into enclosed in-plane domains with nanometric size due to the enhancement of the planar magnetic anisotropy. The spontaneous generation of the biskyrmion lattice and its evolution along different crystal orientations demonstrate the crucial role of intrinsic bi-anisotropy and demagnetization effects. This discovery provides a fundamental insight into the nature of topological magnetic textures in easy-plane anisotropy materials and suggests an arena to explore the topological states in rare-earth magnets as well as their applications in spintronics.

The In Situ Optimization of Spinterface in Polymer Spin Valve by Electronic Phase Separated Oxides.

Tailoring the interface between organic semiconductor (OSC) and ferromagnetic (FM) electrodes, that is, the spinterface, offers a promising way to manipulate and optimize the magnetoresistance (MR) ratio of the organic spin valve (OSV) devices. However, the non-destructive in situ regulation method of spinterface is seldom reported, limiting its theoretical research and further application in organic spintronics. (La2/3 Pr1/3 )5/8 Ca3/8 MnO3 (LPCMO), a recently developed FM material, exhibits a strong electronic phase separation (EPS) property, and can be employed as an effective in situ spinterface adjuster. Herein, we fabricated a LPCMO-based polymer spin valve with a vertical configuration of LPCMO/poly(3-hexylthiophene-2,5-diyl) (P3HT)/Co, and emphasized the important role of LPCMO/P3HT spinterface in MR regulation. A unique competitive spin-scattering mechanism generated by the EPS characteristics of LPCMO inside the polymer spin valve was discovered by abstracting the anomalous non-monotonic MR value as a function of pre-set magnetic field (Bpre ) and temperature (T). Particularly, a record-high MR ratio of 93% was achieved in polymer spin valves under optimal conditions. These findings highlight the importance of interdisciplinary research between organic spintronics and EPS oxides and offer a novel scenario for multi-level storage via spinterface manipulation.

A Distinct Spin Structure and Giant Baromagnetic Effect in MnNiGe Compounds with Fe-Doping.

Spin structure of a magnetic system results from the competition of various exchange couplings. Pressure-driven spin structure evolution, through altering interatomic distance, and hence, electronic structure produces baromagnetic effect (BME), which has potential applications in sensor/actuator field. Here, we report a new spin structure(CyS-AFMb) with antiferromagnetic(AFM) nature in Fe-doped Mn0.87Fe0.13NiGe. Neutron powder diffraction (NPD) under in situ hydrostatic pressure and magnetic field was conducted to reveal the spin configuration and its instabilities. We discovered that a pressure higher than 4 kbar can induce abnormal change of Mn(Fe)-Mn(Fe) distances and transform the CyS-AFMb into a conical spiral ferromagnetic(FM) configuration(45°-CoS-FMa) with easily magnetized but shortened magnetic moment by as much as 22%. The observed BME far exceeds previous reports. Our first-principles calculations provide theoretical supports for the enhanced BME. The compressed lattice by pressure favors the 45°-CoS-FMa and significantly broadened 3d bandwidth of Mn(Fe) atoms, which leads to the shortened magnetic moment and evolution of spin structure.

13-Step Total Synthesis of Atropurpuran.

Herein, we report a concise total synthesis of atropurpuran, a unique and synthetically challenging pentacyclic diterpene that bears a tetracyclo[5.3.3.04,9.04,12]-tridecane skeleton that is unprecedented among natural terpenes. This 13-step approach features a strategy that include early stage rapid skeleton formation and the late-stage introduction of reactive functional groups, thus allowed a high overall synthetic efficiency with minimal use of PGs. The key transformations of our work include a facile construction of the spiro[5.5]undecane moiety through an ring-closing enyne metathesis reaction and an efficient formation of the tetracyclo[5.3.3.04,9.04,12]-tridecane scaffold via an regioselective double oxidative dearomatization/intramolecular Diels-Alder reaction cascade. This efficient approach should also inspire further advances in the synthesis of related complex diterpenes and diterpenoid alkaloids.

A full solid-state conceptual magnetocaloric refrigerator based on hybrid regeneration.

The environmental friendliness and high efficiency of magnetocaloric refrigeration make it a promising substitute for vapor compression refrigeration. However, the common use of heat transfer fluid in conventional passive magnetic regenerators (PMRs) and active magnetic regenerators (AMRs) makes only partial materials contribute to the regeneration process, which produces large regeneration loss and greatly limits the regeneration efficiency and refrigeration performance at high frequency. Herein, we propose a new conceptual hybrid magnetic regenerator (HMR) composed of multiple solid-state high thermal conductivity materials (HTCMs) and magnetocaloric materials (MCMs), in which both HTCM and MCM elements participate in the regeneration process. This novel working mode could greatly reduce regeneration losses caused by dead volume, pressure losses, and temperature nonuniformity in heat transfer substances to markedly improve regeneration efficiency at high working frequencies. Using the experimentally obtained adiabatic temperature change and magnetic work and with the help of finite element simulation, a maximum temperature of 26 K, a dramatically large cooling power of 8.3 kW/kg, and a maximum ideal exergy efficiency of 54.2% are achieved at the working frequency of 10 Hz for an ideal prototype device of a rotary HMR magnetocaloric refrigerator, which shows potential for achieving an integrative, advanced performance against current AMR/PMR systems.

Electron-Assisted Generation and Straight Movement of Skyrmion Bubble in Kagome TbMn6Sn6.

Topological magnetic textures are promising candidates as binary data units for the next-generation memory device. The precise generation and convenient control of nontrivial spin topology at zero field near room temperature endows the critical advantages in skyrmionic devices but is not simultaneously integrated into one material. Here, in the Kagome plane of quantum TbMn6Sn6, the expedient generation of the skyrmion bubbles in versatile forms of lattice, chain, and isolated one by converging the electron beam, where the electron intensity gradient contributes to the dynamic generation from local anisotropy variation near spin reorientation transition (SRT) is reported. Encouragingly, by utilizing the dynamic shift of the SRT domain interface, the straight movement is actualized with the skyrmion bubble slave to the SRT domain interface forming an elastic composite object, avoiding the usual deflection from the skyrmion Hall effect. The critical contribution of the SRT domain interface via conveniently electron-assisted heating is further theoretically validated in micromagnetic simulation, highlighting the compatible application possibility in advanced devices.

Low pressure reversibly driving colossal barocaloric effect in two-dimensional vdW alkylammonium halides.

Plastic crystals as barocaloric materials exhibit the large entropy change rivalling freon, however, the limited pressure-sensitivity and large hysteresis of phase transition hinder the colossal barocaloric effect accomplished reversibly at low pressure. Here we report reversible colossal barocaloric effect at low pressure in two-dimensional van-der-Waals alkylammonium halides. Via introducing long carbon chains in ammonium halide plastic crystals, two-dimensional structure forms in (CH3-(CH2)n-1)2NH2X (X: halogen element) with weak interlayer van-der-Waals force, which dictates interlayer expansion as large as 13% and consequently volume change as much as 12% during phase transition. Such anisotropic expansion provides sufficient space for carbon chains to undergo dramatic conformation disordering, which induces colossal entropy change with large pressure-sensitivity and small hysteresis. The record reversible colossal barocaloric effect with entropy change ΔSr ~ 400 J kg-1 K-1 at 0.08 GPa and adiabatic temperature change ΔTr ~ 11 K at 0.1 GPa highlights the design of novel barocaloric materials by engineering the dimensionality of plastic crystals.

Spontaneous Topological States and Their Mutual Transformations in a Rare-Earth Ferrimagnet.

Nontrivial chiral spin textures with nanometric sizes and novel characteristics (e.g., magnetic skyrmions) are promising for encoding information bits in future energy-efficient and high-density spintronic devices. Because of antiferromagnetic exchange coupling, skyrmions in ferrimagnetic materials exhibit many advantages in terms of size and efficient manipulation, which allow them to overcome the limitations of ferromagnetic skyrmions. Despite recent progress, ferrimagnetic skyrmions have been observed only in few films in the presence of external fields, while those in ferrimagnetic bulks remain elusive. This study reports on spontaneously generated zero-field ground-state magnetic skyrmions and their subsequent transformation into traditional magnetic bubbles via intermediate states of (bi-)target bubbles during a magnetic anisotropy change in the rare-earth ferrimagnetic crystal DyFe11 Ti. Spontaneous reversible topological transformation driven by a temperature-induced spin reorientation transition is directly distinguished using Lorentz transmission electron microscopy. The spontaneous generation of magnetic skyrmions and successive topological transformations in ferrimagnetic DyFe11 Ti are expected to advance the design of topological spin textures with versatile properties and potential applications in rare-earth magnets.

Discovery of Topological Magnetic Textures near Room Temperature in Quantum Magnet TbMn6 Sn6.

The study of topology in quantum materials has fundamentally advanced the understanding in condensed matter physics and potential applications in next-generation quantum information technology. Recently, the discovery of a topological Chern phase in the spin-orbit-coupled Kagome lattice TbMn6 Sn6 has attracted considerable interest. Whereas these phenomena highlight the contribution of momentum space Berry curvature and Chern gap on the electronic transport properties, less is known about the intrinsic real space magnetic texture, which is crucial for understanding the electronic properties and further exploring the unique quantum behavior. Here, the stabilization of topological magnetic skyrmions in TbMn6 Sn6 using Lorentz transmission electron microscopy near room temperature, where the spins experience full spin reorientation transition between the a- and c-axes, is directly observed. An effective spin Hamiltonian based on the Ginzburg-Landau theory is constructed and micromagnetic simulation is performed to clarify the critical role of Ruderman-Kittel-Kasuya-Yosida interaction on the stabilization of skyrmion lattice. These results not only uncover nontrivial spin topological texture in TbMn6 Sn6 , but also provide a solid basis to study its interplay with electronic topology.

Significant Zero Thermal Expansion Via Enhanced Magnetoelastic Coupling in Kagome Magnets.

Zero-thermal-expansion (ZTE) alloys, as dimensionally stable materials, are urgently required in many fields, particularly in highly advanced modern industries. In this study, high-performance ZTE with a negligible coefficient of thermal expansion av as small as 2.4 ppm K-1 in a broad temperature range of 85-245 K is discovered in Hf0.85 Ta0.15 Fe2 C0.01 magnet. It is demonstrated that the addition of trace interstitial atom C into Ta-substituted Hf0.85 Ta0.15 Fe2 exhibits significant capability to tune the normal positive thermal expansion into high-performance ZTE via enhanced magnetoelastic coupling in stabilized ferromagnetic structure. Moreover, direct observation of the magnetic transition between ferromagnetic and triangular antiferromagnetic states via Lorentz transmission electron microscopy, along with corresponding theoretical calculations, further uncovers the manipulation mechanism of ZTE and negative thermal expansion. A convenient and effective method to optimize thermal expansion and achieve ZTE with interstitial C addition may result in broadened applications based on the strong correlation between the magnetic properties and crystal structure.

Classification and Prediction of Skyrmion Material Based on Machine Learning.

The discovery and study of skyrmion materials play an important role in basic frontier physics research and future information technology. The database of 196 materials, including 64 skyrmions, was established and predicted based on machine learning. A variety of intrinsic features are classified to optimize the model, and more than a dozen methods had been used to estimate the existence of skyrmion in magnetic materials, such as support vector machines, k-nearest neighbor, and ensembles of trees. It is found that magnetic materials can be more accurately divided into skyrmion and non-skyrmion classes by using the classification of electronic layer. Note that the rare earths are the key elements affecting the production of skyrmion. The accuracy and reliability of random undersampling bagged trees were 87.5% and 0.89, respectively, which have the potential to build a reliable machine learning model from small data. The existence of skyrmions in LaBaMnO is predicted by the trained model and verified by micromagnetic theory and experiments.

Correlation between evolution of resistive switching and oxygen vacancy configuration in La0.5Ca0.5MnO3 based memristive devices.

We here report a study of the correlation between the evolution of resistive switching and the oxygen vacancy configuration in La0.5Ca0.5MnO3 (LCMO) based memristive devices. By taking advantage of LCMO located at a phase boundary of the metal-to-insulator transition, we observe the development of the high resistive states, depending upon not only the electrical pulse magnitude but also the switching cycles. We discuss the experimental results by an oxygen migration model that involves both single isolated and clustered oxygen vacancies, which are later verified using aberration-corrected scanning transmission electron microscopy.

Enhanced Performance of ΔTad upon Frequent Alternating Magnetic Fields in FeRh Alloys by Introducing Second Phases.

The cyclability and frequency dependence of the adiabatic temperature change (ΔTad) under an alternating magnetic field (AMF) are significantly important from the viewpoint of refrigeration application. Our studies demonstrated, by direct measurements, that the cyclability and low-magnetic-field performance of ΔTad in FeRh alloys can be largely enhanced by introducing second phases. The ΔTad under a 1.8 T, 0.13 Hz AMF is reduced by 14%, which is much better than that (40-50%) of monophase FeRh previously reported. More importantly, the introduction of second phases enables the antiferromagnetic-ferromagnetic phase transition to be driven by a lower magnetic field. Thus, ΔTad is significantly enhanced under a 0.62 T, 1 Hz AMF, and its value is 70% larger than that of monophase FeRh previously reported. Although frequency dependence of ΔTad occurs, the specific cooling power largely increases by 11 times from 0.17 to 1.9 W/g, as the frequency increases from 1 to 18.4 Hz under an AMF of 0.62 T. Our analysis of the phase transition dynamics based on magnetic relaxation measurements indicates that the activation energy barrier is lowered owing to the existence of second phases in FeRh alloys, which should be responsible for the reduction of the driving field. This work provides an effective way to enhance the cyclability and low-magnetic-field performance of ΔTad under an AMF in FeRh alloys by introducing second phases.

Compressive-Strain-Facilitated Fast Oxygen Migration with Reversible Topotactic Transformation in La0.5Sr0.5CoOx via All-Solid-State Electrolyte Gating.

Modifying the crystal structure and corresponding functional properties of complex oxides by regulating their oxygen content has promising applications in energy conversion and chemical looping, where controlling oxygen migration plays an important role. Therefore, finding an efficacious and feasible method to facilitate oxygen migration has become a critical requirement for practical applications. Here, we report a compressive-strain-facilitated oxygen migration with reversible topotactic phase transformation (RTPT) in La0.5Sr0.5CoOx films based on all-solid-state electrolyte gating modulation. With the lattice strain changing from tensile to compressive strain, significant reductions in modulation duration (∼72%) and threshold voltage (∼70%) for the RTPT were observed, indicating great promotion of RTPT by compressive strain. Density functional theory calculations verify that such compressive-strain-facilitated efficient RTPT comes from significant reduction of the oxygen migration barrier in compressive-strained films. Further, ac-STEM, EELS, and sXAS investigations reveal that varying strain from tensile to compressive enhances the Co 3d band filling, thereby suppressing the Co-O hybrid bond in oxygen vacancy channels, elucidating the micro-origin of such compressive-strain-facilitated oxygen migration. Our work suggests that controlling electronic orbital occupation of Co ions in oxygen vacancy channels may help facilitate oxygen migration, providing valuable insights and practical guidance for achieving highly efficient oxygen-migration-related chemical looping and energy conversion with complex oxides.

Large Low-Field Magnetoresistance (LFMR) Effect in Free-Standing La0.7Sr0.3MnO3 Films.

The realization of a large low-field magnetoresistance (LFMR) effect in free-standing magnetic oxide films is a crucial goal toward promoting the development of flexible, low power consumption, and nonvolatile memory devices for information storage. La0.7Sr0.3MnO3 (LSMO) is an ideal material for spintronic devices due to its excellent magnetic and electronic properties. However, it is difficult to achieve both a large LFMR effect and high flexibility in LSMO films due to the lack of research on LFMR-related mechanisms and the strict LSMO growth conditions, which require rigid substrates. Here, we induced a large LFMR effect in an LSMO/mica heterostructure by utilizing a disorder-related spin-polarized tunneling effect and developed a simple transfer method to obtain free-standing LSMO films for the first time. Electrical and magnetic characterizations of these free-standing LSMO films revealed that all of the principal properties of LSMO were sustained under compressive and tensile conditions. Notably, the magnetoresistance of the processed LSMO film reached up to 16% under an ultrasmall magnetic field (0.1 T), which is 80 times that of a traditional LSMO film. As a demonstration, a stable nonvolatile multivalue storage function in flexible LSMO films was successfully achieved. Our work may pave the way for future wearable resistive memory device applications.

Field-free topological behavior in the magnetic domain wall of ferrimagnetic GdFeCo.

Exploring and controlling topological textures such as merons and skyrmions has attracted enormous interests from the perspective of fundamental research and spintronic applications. It has been predicted theoretically and proved experimentally that the lattice form of topological meron-skyrmion transformation can be realized with the requirement of external magnetic fields in chiral ferromagnets. However, such topological transition behavior has yet to be verified in other materials. Here, we report real-space observation of magnetic topology transformation between meron pairs and skyrmions in the localized domain wall of ferrimagnetic GdFeCo films without the need of magnetic fields. The topological transformation in the domain wall of ferrimagnet is introduced by temperature-induced spin reorientation transition (SRT) and the underlying mechanism is revealed by micromagnetic simulations. The convenient electric-controlling topology transformation and driving motion along the confined domain wall is further anticipated, which will enable advanced application in magnetic devices.

Spontaneous Topological Magnetic Transitions in NdCo5 Rare-Earth Magnets.

Particle-like magnetic textures with nanometric sizes, such as skyrmions, are potentially suitable for designing high-efficiency information bits in future spintronics devices. In general, the Dzyaloshinskii-Moriya interactions and dipolar interactions are the dominant factors for generating nonlinear spin configurations. However, to stabilize the topological skyrmions, an external magnetic field is usually required. In this study, the spontaneous emergence of skyrmions is directly observed, together with the unique successive topological domain evolution during the spin reorientation transition in a neodymium-cobalt (NdCo5 ) rare-earth magnet. On decreasing the temperature, nanometric skyrmion lattices evolve into enclosed in-plane domains (EIPDs) similar to mini bar-magnets with size below 120 nm. The internal magnetization rotates with magnetic anisotropy, demonstrating the ability to manipulate the mini bar-magnets. The nanoscale EIPD lattices remain robust over the wide temperature range of 241-167 K, indicating the possibility of high-density in-plane magnetic information storage. The generation of spontaneous magnetic skyrmions and the successive domain transformation in the traditional NdCo5 rare-earth magnet may prompt application exploration for topological magnetic spin textures with novel physical mechanisms in versatile magnets.

Spontaneous (Anti)meron Chains in the Domain Walls of van der Waals Ferromagnetic Fe5- x GeTe2.

The promise of topologically vortex-like magnetic spin textures hinges on the intriguing physical properties and theories in fundamental research and their distinguished roles as high-efficiency information units in future spintronics. The exploration of such magnetic states with unique spin configurations has never ceased. In this study, the emergence of unconventional (anti)meron chains from a domain wall pair is directly observed at zero field in 2D ferromagnetic Fe5- x GeTe2 , closely correlated with significant enhancement of the in-plane magnetization and weak van der Waals interactions. The simultaneous appearance of a large topological Hall effect is observed at the same temperature range as that of the abnormal magnetic transition. Moreover, the distinctive features of the (anti)meron chains and their collective dynamic behavior under external fields may provide concrete experimental evidence for the recent theoretical prediction of the magnetic-domain-wall topology and endorse a broader range of possibilities for electronics, spintronics, condensed matter physics, etc.

In situ TEM study on diversified martensitic transition behaviour in Ni50Mn35In15 alloys.

Ni-Mn-In magnetic shape-memory alloys are attractive materials due to their important functional properties relating to the martensitic transition. Understanding the complex martensitic magnetism and the transition process is of crucial importance not only from a fundamental but also from a technological point of view. Here, we demonstrate the dynamic magnetic domains and microstructures during the martensitic transition in the bulk and melt-spun ribbons of Ni50Mn35In15via in situ Lorentz transmission electron microscopy. The significant evolutionary differences in correlation with the temperature dependence of magnetization are identified between the bulk and ribbons. For a bulk alloy with L21 crystal structure at room temperature, the complete martensite with 7 M modulation in the paramagnetic state and the successive stripe magnetic domains in ferromagnetic martensite develop with a further decrease in the temperature. The stripe domains evolve into biskyrmion-like spin configurations when a perpendicular magnetic field is applied. In contrast, the partial austenitic phase always coexists with the martensitic phase in the ribbons even far below the martensitic transition temperatures and the martensitic phase presents a dominant twinning stack morphology with 5 M modulation and various magnetic domains. During the subsequent reheating-cooling cycles, the thermal hysteresis behavior and the transition reversibility in the bulk and ribbons are represented via the microstructural evolution.