Hopfion rings in a cubic chiral magnet.

Magnetic skyrmions and hopfions are topological solitons1-well-localized field configurations that have gained considerable attention over the past decade owing to their unique particle-like properties, which make them promising objects for spintronic applications. Skyrmions2,3 are two-dimensional solitons resembling vortex-like string structures that can penetrate an entire sample. Hopfions4-9 are three-dimensional solitons confined within a magnetic sample volume and can be considered as closed twisted skyrmion strings that take the shape of a ring in the simplest case. Despite extensive research on magnetic skyrmions, the direct observation of magnetic hopfions is challenging10 and has only been reported in a synthetic material11. Here we present direct observations of hopfions in crystals. In our experiment, we use transmission electron microscopy to observe hopfions forming coupled states with skyrmion strings in B20-type FeGe plates. We provide a protocol for nucleating such hopfion rings, which we verify using Lorentz imaging and electron holography. Our results are highly reproducible and in full agreement with micromagnetic simulations. We provide a unified skyrmion-hopfion homotopy classification and offer insight into the diversity of topological solitons in three-dimensional chiral magnets.

Ultrabroadband plasmon driving selective photoreforming of methanol under ambient conditions.

Liquid methanol has the potential to be the hydrogen energy carrier and storage medium for the future green economy. However, there are still many challenges before zero-emission, affordable molecular H2 can be extracted from methanol with high performance. Here, we present noble-metal-free Cu-WC/W plasmonic nanohybrids which exhibit unsurpassed solar H2 extraction efficiency from pure methanol of 2,176.7 µmol g-1 h-1 at room temperature and normal pressure. Macro-to-micro experiments and simulations unveil that local reaction microenvironments are generated by the coperturbation of WC/W's lattice strain and infrared-plasmonic electric field. It enables spontaneous but selective zero-emission reaction pathways. Such microenvironments are found to be highly cooperative with solar-broadband-plasmon-excited charge carriers flowing from Cu to WC surfaces for efficient stable CH3OH plasmonic reforming with C3-dominated liquid products and 100% selective gaseous H2. Such high efficiency, without any COx emission, can be sustained for over a thousand-hour operation without obvious degradation.

Field-Free Switching of Perpendicular Magnetization in an Ultrathin Epitaxial Magnetic Insulator.

For energy-efficient magnetic memories, switching of perpendicular magnetization by spin-orbit torque (SOT) appears to be a promising solution. This SOT switching requires the assistance of an in-plane magnetic field to break the symmetry. Here, we demonstrate the field-free SOT switching of a perpendicularly magnetized thulium iron garnet (Tm3Fe5O12, TmIG). The polarity of the switching loops, clockwise or counterclockwise, is determined by the direction of the initial current pulses, in contrast with field-assisted switching where the polarity is controlled by the direction of the magnetic field. From Brillouin light scattering, we determined the Dzyaloshinskii-Moriya interaction (DMI) induced by the Pt-TmIG interface. We will discuss the possible origins of field-free switching and the roles of the interfacial DMI and cubic magnetic anisotropy of TmIG. This discussion is substantiated by magnetotransport, Kerr microscopy, and micromagnetic simulations. Our observation of field-free electrical switching of a magnetic insulator is an important milestone for low-power spintronic devices.

Live Iterative Ptychography.

We demonstrate live-updating ptychographic reconstruction with the extended ptychographical iterative engine, an iterative ptychography method, during ongoing data acquisition. The reconstruction starts with a small subset of the total data, and as the acquisition proceeds the data used for reconstruction are extended. This creates a live-updating view of object and illumination that allows monitoring the ongoing experiment and adjusting parameters with quick turn around. This is particularly advantageous for long-running acquisitions. We show that such a gradual reconstruction yields interpretable results already with a small subset of the data. We show simulated live processing with various scan patterns, parallelized reconstruction, and real-world live processing at the hard X-ray ptychographic nanoanalytical microscope PtyNAMi at the PETRA III beamline.

Nanoscale Three-Dimensional Charge Density and Electric Field Mapping by Electron Holographic Tomography.

The operation of nanoscale electronic devices is related intimately to the three-dimensional (3D) charge density distributions within them. Here, we demonstrate the quantitative 3D mapping of the charge density and long-range electric field associated with an electrically biased carbon fiber nanotip with a spatial resolution of approximately 5 nm using electron holographic tomography in the transmission electron microscope combined with model-based iterative reconstruction. The approach presented here can be applied to a wide range of other nanoscale materials and devices.

Large Interfacial Rashba Interaction Generating Strong Spin-Orbit Torques in Atomically Thin Metallic Heterostructures.

The hallmark of spintronics has been the ability of spin-orbit interactions to convert a charge current into a spin current and vice versa, mainly in the bulk of heavy metal thin films. Here, we demonstrate how a light metal interface profoundly affects both the nature of spin-orbit torques and its efficiency in terms of damping-like (HDL) and field-like (HFL) effective fields in ultrathin Co films. We measure unexpectedly HFL/HDL ratios much larger than 1 by inserting a nanometer-thin Al metallic layer in Pt|Co|Al|Pt as compared to a similar stacking, including Cu as a reference. From our modeling, these results evidence the existence of large Rashba interaction at the Co|Al interface generating a giant HFL, which is not expected from a metallic interface. The occurrence of such enhanced torques from an interfacial origin is further validated by demonstrating current-induced magnetization reversal showing a significant decrease of the critical current for switching.

Element-Specific Study of Magnetic Anisotropy and Hardening in SmCo5-xCux Thin Films.

This work investigates the effect of copper substitution on the magnetic properties of SmCo5 thin films synthesized by molecular beam epitaxy. A series of thin films with varying concentrations of Cu were grown under otherwise identical conditions to disentangle structural and compositional effects on the magnetic behavior. The combined experimental and theoretical studies show that Cu substitution at the Co3g sites not only stabilizes the formation of the SmCo5 structure but also enhances magnetic anisotropy and coercivity. Density functional theory calculations indicate that Sm(Co4Cu3g)5 possesses a higher single-ion anisotropy as compared to pure SmCo5. In addition, X-ray magnetic circular dichroism reveals that Cu substitution causes an increasing decoupling of the Sm 4f and Co 3d moments. Scanning transmission electron microscopy confirms predominantly SmCo5 phase formation and reveals nanoscale inhomogeneities in the Cu and Co distribution. Our study based on thin film model systems and advanced characterization as well as modeling reveals novel aspects of the complex interplay of intrinsic and extrinsic contributions to magnetic hysteresis in rare-earth-based magnets, i.e., the combination of increased intrinsic anisotropy due to Cu substitution and the extrinsic effect of inhomogeneous elemental distribution of Cu and Co.

Wigner Distribution Deconvolution Adaptation for Live Ptychography Reconstruction.

We propose a modification of Wigner distribution deconvolution (WDD) to support live processing ptychography. Live processing allows to reconstruct and display the specimen transmission function gradually while diffraction patterns are acquired. For this purpose, we reformulate WDD and apply a dimensionality reduction technique that reduces memory consumption and increases processing speed. We show numerically that this approach maintains the reconstruction quality of specimen transfer functions as well as reduces computational complexity during acquisition processes. Although we only present the reconstruction for scanning transmission electron microscopy datasets, in general, the live processing algorithm we present in this paper can be applied to real-time ptychographic reconstruction for different fields of application.

Counting Point Defects at Nanoparticle Surfaces by Electron Holography.

Metal oxide nanoparticles exhibit outstanding catalytic properties, believed to be related to the presence of oxygen vacancies at the particle's surface. However, little quantitative information is known about concentrations of point defects inside and at surfaces of these nanoparticles, due to the challenges in achieving an atomically resolved experimental access. By employing off-axis electron holography, we demonstrate, using MgO nanoparticles as an example, a methodology that discriminates between mobile charge induced by electron beam irradiation and immobile charge associated with deep traps induced by point defects as well as distinguishes between bulk and surface point defects. Counting the immobile charge provides a quantification of the concentration of F2+ centers induced by oxygen vacancies at the MgO nanocube surfaces.

Multilayered Ceramic Membrane with Ion Conducting Thin Layer Induced by Interface Reaction for Stable Hydrogen Production.

Conventional methods for fabricating multilayered ceramic membranes with ion conducting dense thin layers are often cumbersome, costly, and limited by poor adhesion between layers. Inspired by the architectural structure of the rooted grasses in soil, here, we report an interface-reaction-induced reassembly approach for the direct fabrication of Ce0.9 Gd0.1 O2-δ (CGO) thin layers rooted in the parent multilayered ceramic membranes by only one firing step. The CGO dense layers are very thin, and adhered strongly to the parent support layer, ensuring low ionic transport resistance and structural integrity of the multilayered membranes. When using as an oxygen permeable membrane for upgrading fossil-fuel-derived hydrogen, it shows very long durability in harsh conditions containing H2 O, CH4 , H2 , CO2 and H2 S. Furthermore, our approach is highly scalable and applicable to a wide variety of ion conducting thin layers, including Y0.08 Zr0.92 O2-δ , Ce0.9 Sm0.1 O2-δ and Ce0.9 Pr0.1 O2-δ .

Electrostatic Shaping of Magnetic Transition Regions in La_{0.7}Sr_{0.3}MnO_{3}.

We report a magnetic transition region in La_{0.7}Sr_{0.3}MnO_{3} with gradually changing magnitude of magnetization, but no rotation, stable at all temperatures below T_{C}. Spatially resolved magnetization, composition and Mn valence data reveal that the magnetic transition region is induced by a subtle Mn composition change, leading to charge transfer at the interface due to carrier diffusion and drift. The electrostatic shaping of the magnetic transition region is mediated by the Mn valence, which affects both magnetization by Mn^{3+}-Mn^{4+} double exchange interaction and free carrier concentration.

Automatic Alignment of an Orbital Angular Momentum Sorter in a Transmission Electron Microscope Using a Convolutional Neural Network.

We report on the automatic alignment of a transmission electron microscope equipped with an orbital angular momentum sorter using a convolutional neural network. The neural network is able to control all relevant parameters of both the electron-optical setup of the microscope and the external voltage source of the sorter without input from the user. It can compensate for mechanical and optical misalignments of the sorter, in order to optimize its spectral resolution. The alignment is completed over a few frames and can be kept stable by making use of the fast fitting time of the neural network.

Discovery and Implications of Hidden Atomic-Scale Structure in a Metallic Meteorite.

Iron and its alloys have made modern civilization possible, with metallic meteorites providing one of the human's earliest sources of usable iron as well as providing a window into our solar system's billion-year history. Here highest-resolution tools reveal the existence of a previously hidden FeNi nanophase within the extremely slowly cooled metallic meteorite NWA 6259. This new nanophase exists alongside Ni-poor and Ni-rich nanoprecipitates within a matrix of tetrataenite, the uniaxial, chemically ordered form of FeNi. The ferromagnetic nature of the nanoprecipitates combined with the antiferromagnetic character of the FeNi nanophases gives rise to a complex magnetic state that evolves dramatically with temperature. These observations extend and possibly alter our understanding of celestial metallurgy, provide new knowledge concerning the archetypal Fe-Ni phase diagram and supply new information for the development of new types of sustainable, technologically critical high-energy magnets.

Single-particle cryo-EM: alternative schemes to improve dose efficiency.

Imaging of biomolecules by ionizing radiation, such as electrons, causes radiation damage which introduces structural and compositional changes of the specimen. The total number of high-energy electrons per surface area that can be used for imaging in cryogenic electron microscopy (cryo-EM) is severely restricted due to radiation damage, resulting in low signal-to-noise ratios (SNR). High resolution details are dampened by the transfer function of the microscope and detector, and are the first to be lost as radiation damage alters the individual molecules which are presumed to be identical during averaging. As a consequence, radiation damage puts a limit on the particle size and sample heterogeneity with which electron microscopy (EM) can deal. Since a transmission EM (TEM) image is formed from the scattering process of the electron by the specimen interaction potential, radiation damage is inevitable. However, we can aim to maximize the information transfer for a given dose and increase the SNR by finding alternatives to the conventional phase-contrast cryo-EM techniques. Here some alternative transmission electron microscopy techniques are reviewed, including phase plate, multi-pass transmission electron microscopy, off-axis holography, ptychography and a quantum sorter. Their prospects for providing more or complementary structural information within the limited lifetime of the sample are discussed.

Engineering stable electrocatalysts by synergistic stabilization between carbide cores and Pt shells.

Core-shell particles with earth-abundant cores represent an effective design strategy for improving the performance of noble metal catalysts, while simultaneously reducing the content of expensive noble metals1-4. However, the structural and catalytic stabilities of these materials often suffer during the harsh conditions encountered in important reactions, such as the oxygen reduction reaction (ORR)3-5. Here, we demonstrate that atomically thin Pt shells stabilize titanium tungsten carbide cores, even at highly oxidizing potentials. In situ, time-resolved experiments showed how the Pt coating protects the normally labile core against oxidation and dissolution, and detailed microscopy studies revealed the dynamics of partially and fully coated core-shell nanoparticles during potential cycling. Particles with complete Pt coverage precisely maintained their core-shell structure and atomic composition during accelerated electrochemical ageing studies consisting of over 10,000 potential cycles. The exceptional durability of fully coated materials highlights the potential of core-shell architectures using earth-abundant transition metal carbide (TMC) and nitride (TMN) cores for future catalytic applications.

Three-Dimensional Measurement of Magnetic Moment Vectors Using Electron Magnetic Chiral Dichroism at Atomic Scale.

Here we have developed an approach of three-dimensional (3D) measurement of magnetic moment vectors in three Cartesian directions using electron magnetic chiral dichroism (EMCD) at atomic scale. Utilizing a subangstrom convergent electron beam in the scanning transmission electron microscopy (STEM), beam-position-dependent chiral electron energy-loss spectra (EELS), carrying the EMCD signals referring to magnetization in three Cartesian directions, can be obtained during the scanning across the atomic planes. The atomic resolution EMCD signals from all of three directions can be separately obtained simply by moving the EELS detector. Moreover, the EMCD signals can be remarkably enhanced using a defocused electron beam, relieving the issues of low signal intensity and signal-to-noise-ratio especially at atomic resolution. Our proposed method is compatible with the setup of the widely used atomic resolution STEM-EELS technique and provides a straightforward way to achieve 3D magnetic measurement at atomic scale on newly developing magnetic-field-free TEM.

Experimental Demonstration of an Electrostatic Orbital Angular Momentum Sorter for Electron Beams.

The component of orbital angular momentum (OAM) in the propagation direction is one of the fundamental quantities of an electron wave function that describes its rotational symmetry and spatial chirality. Here, we demonstrate experimentally an electrostatic sorter that can be used to analyze the OAM states of electron beams in a transmission electron microscope. The device achieves postselection or sorting of OAM states after electron-material interactions, thereby allowing the study of new material properties such as the magnetic states of atoms. The required electron-optical configuration is achieved by using microelectromechanical systems technology and focused ion beam milling to control the electron phase electrostatically with a lateral resolution of 50 nm. An OAM resolution of 1.5ℏ is realized in tests on controlled electron vortex beams, with the perspective of reaching an optimal OAM resolution of 1ℏ in the near future.

Visualizing Magnetic Structure in 3D Nanoscale Ni-Fe Gyroid Networks.

Arrays of interacting 2D nanomagnets display unprecedented electromagnetic properties via collective effects, demonstrated in artificial spin ices and magnonic crystals. Progress toward 3D magnetic metamaterials is hampered by two challenges: fabricating 3D structures near intrinsic magnetic length scales (sub-100 nm) and visualizing their magnetic configurations. Here, we fabricate and measure nanoscale magnetic gyroids, periodic chiral networks comprising nanowire-like struts forming three-connected vertices. Via block copolymer templating, we produce Ni75Fe25 single-gyroid and double-gyroid (an inversion pair of single-gyroids) nanostructures with a 42 nm unit cell and 11 nm diameter struts, comparable to the exchange length in Ni-Fe. We visualize their magnetization distributions via off-axis electron holography with nanometer spatial resolution and interpret the patterns using finite-element micromagnetic simulations. Our results suggest an intricate, frustrated remanent state which is ferromagnetic but without a unique equilibrium configuration, opening new possibilities for collective phenomena in magnetism, including 3D magnonic crystals and unconventional computing.

Structural perspective on revealing heat dissipation behavior of CoFe2O4-Pd nanohybrids: great promise for magnetic fluid hyperthermia.

Loss mechanisms in fluid heating of cobalt ferrite (CFO) nanoparticles and CFO-Pd heterodimer colloidal suspensions are investigated as a function of particle size, fluid concentration and magnetic field amplitude. The specific absorption rate (SAR) is found to vary with increasing particle size due to a change in dominant heating mechanism from susceptibility to hysteresis and frictional loss. The maximum SAR is obtained for particle diameters of 11-15 nm as a result of synergistic contributions of susceptibility loss, including Néel and Brownian relaxation and especially hysteresis loss, thereby validating the applicability of linear response theory to superparamagnetic CFO nanoparticles. Our results show that the ferrofluid concentration and magnetic field amplitude alter interparticle interactions and associated heating efficiency. The SAR of the CFO nanoparticles could be maximized by adjusting the synthesis parameters. Despite the paramagnetic properties of individual palladium nanoparticles, CFO-Pd heterodimer suspensions were observed to have surprisingly improved magnetization as well as SAR values, when compared with CFO ferrofluids. This difference is attributed to interfacial interactions between the magnetic moments of paramagnetic Pd and superparamagnetic/ferrimagnetic CFO. SAR values measured from CFO-Pd heterodimer suspensions were found to be 47-52 W gFerrite-1, which is up to a factor of two higher than the SAR values of commercially available ferrofluids, demonstrating their potential as efficient heat mediators. Our results provide insight into the utilization of CFO-Pd heterodimer suspensions as potential nanoplatforms for diagnostic and therapeutic biomedical applications, e.g., in cancer hyperthermia, cryopreserved tissue warming, thermoablative therapy, drug delivery and bioimaging.

Magnetic quantification of single-crystalline Fe and Co nanowires via off-axis electron holography.

Investigating the local micromagnetic structure of ferromagnetic nanowires (NWs) at the nanoscale is essential to study the structure-property relationships and can facilitate the design of nanostructures for technology applications. Herein, we synthesized high-quality iron and cobalt NWs and investigated the magnetic properties of these NWs using off-axis electron holography. The Fe NWs are about 100 nm in width and a few micrometers in length with a preferential growth direction of [100], while the Co NWs have a higher aspect-ratio with preferential crystal growth along the [110] direction. It is noted that compact passivation surface layers of oxides protect these NWs from further oxidation, even after nearly two years of exposure to ambient conditions; furthermore, these NWs display homogeneous ferromagnetism along their axial direction revealing the domination of shape anisotropy on magnetic behavior. Importantly, the average value of magnetic induction strengths of Fe NWs (2.07 {±} 0.10 T) and Co NWs (1.83 {±} 0.15 T) is measured to be very close to the respective theoretical value, and it shows that the surface oxide layers do not affect the magnetic moments in NWs. Our results provide a useful synthesis approach for the fabrication of single-crystalline, defect-free metal NWs and give insight into the micromagnetic properties in ferromagnetic NWs based on the transmission electron microscopy measurements.