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The last decade has seen significant improvements in our understanding of skyrmions current induced dynamics, along with their room temperature stabilization, however, the impact of local material inhomogeneities still remains an issue that impedes reaching the regime of steady state motion of these spin textures. Here, we study the spin-torque driven motion of skyrmions in synthetic ferrimagnetic multilayers with the aim of achieving high mobility and reduced skyrmion Hall effect. We consider Pt|Co|Tb multilayers of various thicknesses with antiferromagnetic coupling between the Co and Tb magnetization. The increase of Tb thickness in the multilayers reduces the total magnetic moment and increases the spin-orbit torques allowing to reach velocities up to 400 ms -1 for skyrmions with diameters of about 160 nm. We demonstrate that due to reduced skyrmion Hall effect combined with the edge repulsion of the magnetic track, the skyrmions move along the track without any transverse deflection. Further, by comparing the field-induced domain wall motion and current-induced skyrmion motion, we demonstrate that the skyrmions at the largest current densities present all the characteristics of a dynamical flow regime., (© 2024. The Author(s).)

Quantitative interpretation of transmission electron microscopy (TEM) data of crystalline specimens often requires the accurate knowledge of the local crystal orientation. A method is presented which exploits momentum-resolved scanning TEM (STEM) data to determine the local mistilt from a major zone axis. It is based on a geometric analysis of Kikuchi bands within a single diffraction pattern, yielding the center of the Laue circle. Whereas the approach is not limited to convergent illumination, it is here developed using unit-cell averaged diffraction patterns corresponding to high-resolution STEM settings. In simulation studies, an accuracy of approximately 0.1 mrad is found. The method is implemented in automated software and applied to crystallographic tilt and in-plane rotation mapping in two experimental cases. In particular, orientation maps of high-Mn steel and an epitaxially grown La 0.7 Sr 0.3 MnO 3 -SrTiO 3 interface are presented. The results confirm the estimates of the simulation study and indicate that tilt mapping can be performed consistently over a wide field of view with diameters well above 100 nm at unit cell real space sampling., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024. Published by Elsevier B.V.)

Magnetic skyrmions are topologically nontrivial spin configurations that possess particle-like properties. Earlier research has mainly focused on a specific type of skyrmion with topological charge Q = -1. However, theoretical analyses of 2D chiral magnets have predicted the existence of skyrmion bags-solitons with arbitrary positive or negative topological charge. Although such spin textures are metastable states, recent experimental observations have confirmed the stability of isolated skyrmion bags in a limited range of applied magnetic fields. Here, by utilizing Lorentz transmission electron microscopy, the extraordinary stability of skyrmion bags in thin plates of B20-type FeGe is shown. In particular, it is shown that skyrmion bags embedded within a skyrmion lattice remain stable even in zero or inverted external magnetic fields. A robust protocol for nucleating such embedded skyrmion bags is provided. The results agree perfectly with micromagnetic simulations and establish thin plates of cubic chiral magnets as a powerful platform for exploring a broad spectrum of topological magnetic solitons., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

The exchange bias phenomenon, inherent in exchange-coupled ferromagnetic and antiferromagnetic systems, has intrigued researchers for decades. Van der Waals materials, with their layered structures, offer an ideal platform for exploring exchange bias. However, effectively manipulating exchange bias in van der Waals heterostructures remains challenging. This study investigates the origin of exchange bias in MnPS 3 /Fe 3 GeTe 2 van der Waals heterostructures, demonstrating a method to modulate nearly 1000% variation in magnitude through simple thermal cycling. Despite the compensated interfacial spin configuration of MnPS 3 , a substantial 170 mT exchange bias is observed at 5 K, one of the largest observed in van der Waals heterostructures. This significant exchange bias is linked to anomalous weak ferromagnetic ordering in MnPS 3 below 40 K. The tunability of exchange bias during thermal cycling is attributed to the amorphization and changes in the van der Waals gap during field cooling. The findings highlight a robust and adjustable exchange bias in van der Waals heterostructures, presenting a straightforward method to enhance other interface-related spintronic phenomena for practical applications. Detailed interface analysis reveals atom migration between layers, forming amorphous regions on either side of the van der Waals gap, emphasizing the importance of precise interface characterization in these heterostructures., (© 2024 The Author(s). Advanced Materials published by Wiley‐VCH GmbH.)

Ga-doped Li 7 La 3 Zr 2 O 12 garnet solid electrolytes exhibit the highest Li-ion conductivities among the oxide-type garnet-structured solid electrolytes, but instabilities toward Li metal hamper their practical application. The instabilities have been assigned to direct chemical reactions between LiGaO 2 coexisting phases and Li metal by several groups previously. Yet, the understanding of the role of LiGaO 2 in the electrochemical cell and its electrochemical properties is still lacking. Here, we are investigating the electrochemical properties of LiGaO 2 through electrochemical tests in galvanostatic cells versus Li metal and complementary ex situ studies via confocal Raman microscopy, quantitative phase analysis based on powder X-ray diffraction, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, and electron energy loss spectroscopy. The results demonstrate considerable and surprising electrochemical activity, with high reversibility. A three-stage reaction mechanism is derived, including reversible electrochemical reactions that lead to the formation of highly electronically conducting products. The results have considerable implications for the use of Ga-doped Li 7 La 3 Zr 2 O 12 electrolytes in all-solid-state Li-metal battery applications and raise the need for advanced materials engineering to realize Ga-doped Li 7 La 3 Zr 2 O 12 for practical use.

The current-driven movement of magnetic skyrmions along a nanostripe is essential for the advancement and functionality of a new category of spintronic devices resembling racetracks. Despite extensive research into skyrmion dynamics, experimental verification of current-induced motion of ultra-small skyrmions within an ultrathin nanostripe is still pending. Here, we unveil the motion of individual 80 nm-size skyrmions in an FeGe track with an ultrathin width of 100 nm. The skyrmions can move steadily along the track over a broad range of current densities by using controlled pulse durations of as low as 2 ns. The potential landscape, arising from the magnetic edge twists in such a geometrically confined system, introduces skyrmion inertia and ensures efficient motion with a vanishing skyrmion Hall angle. Our results showcase the steady motion of skyrmions in an ultrathin track, offering a practical pathway for implementing skyrmion-based spintronic devices., (© 2024. The Author(s).)

Magnetic skyrmions are quasi-particles with a swirling spin texture that form two-dimensional lattices. Skyrmion lattices can exhibit defects in response to geometric constraints, variations of temperature or applied magnetic fields. Measuring deformations in skyrmion lattices is important to understand the interplay between the lattice structure and external influences. Geometric phase analysis (GPA) is a Fourier-based image processing method that is used to measure deformation fields in high resolution transmission electron microscopy (TEM) images of crystalline materials. Here, we show that GPA can be applied quantitatively to Lorentz TEM images of two-dimensional skyrmion lattices obtained from a chiral magnet of FeGe. First, GPA is used to map deformation fields around a 5-7 dislocation and the results are compared with the linear theory of elasticity. Second, rotation angles between skyrmion crystal grains are measured and compared with angles calculated from the density of dislocations. Third, an orientational order parameter and the corresponding correlation function are calculated to describe the evolution of the disorder as a function of applied magnetic field. The influence of sources of artifacts such as geometric distortions and large defoci are also discussed., (© 2024. The Author(s).)

Concurrent structural and electronic transformations in VO 2 thin films are of 2-fold importance: enabling fine-tuning of the emergent electrical properties in functional devices, yet creating an intricate interfacial domain structure of transitional phases. Despite the importance of understanding the structure of VO 2 thin films, a detailed real-space atomic structure analysis in which the oxygen atomic columns are also resolved is lacking. Moreover, intermediate atomic structures have remained elusive due to the lack of robust atomically resolved quantitative analysis. Here, we directly resolve both V and O atomic columns and discover the presence of intermediate monoclinic (M2) phase nanolayers (less than 2 nm thick) in epitaxially grown VO 2 films on a TiO 2 (001) substrate, where the dominant part of VO 2 undergoes a transition from the tetragonal (rutile) phase to the monoclinic M1 phase. Strain analysis suggests that the presence of the M2 phase is related to local strain gradients near the TiO 2 /VO 2 interface. We unfold the crucial role of imaging the spatial configurations of the oxygen anions (in addition to V cations) by utilizing atomic-resolution electron microscopy. Our approach can be used to unravel the structural transitions in a wide range of correlated oxides, offering substantial implications for, e.g., optoelectronics and ferroelectrics.

High energy density electrochemical systems such as metal batteries suffer from uncontrollable dendrite growth on cycling, which can severely compromise battery safety and longevity. This originates from the thermodynamic preference of metal nucleation on electrode surfaces, where obtaining the crucial information on metal deposits in terms of crystal orientation, plated volume, and growth rate is very challenging. In situ liquid phase transmission electron microscopy (LPTEM) is a promising technique to visualize and understand electrodeposition processes, however a detailed quantification of which presents significant difficulties. Here by performing Zn electroplating and analyzing the data via basic image processing, this work not only sheds new light on the dendrite growth mechanism but also demonstrates a workflow showcasing how dendritic deposition can be visualized with volumetric and growth rate information. These results along with additionally corroborated 4D STEM analysis take steps to access information on the crystallographic orientation of the grown Zn nucleates and toward live quantification of in situ electrodeposition processes., (© 2024 The Authors. Small Methods published by Wiley‐VCH GmbH.)

Two-dimensional van der Waals (vdW) heterostructures are an attractive platform for studying exchange bias due to their defect-free and atomically flat interfaces. Chromium thiophosphate (CrPS 4 ), an antiferromagnetic material, possesses uncompensated magnetic spins in a single layer, rendering it a promising candidate for exploring exchange bias phenomena. Recent findings have highlighted that naturally oxidized vdW ferromagnetic Fe 3 GeTe 2 exhibits exchange bias, attributed to the antiferromagnetic coupling of its ultrathin surface oxide layer (O-FGT) with the underlying unoxidized Fe 3 GeTe 2 . Anomalous Hall measurements are employed to scrutinize the exchange bias within the CrPS 4 /(O-FGT)/Fe 3 GeTe 2 heterostructure. This analysis takes into account the contributions from both the perfectly uncompensated interfacial CrPS 4 layer and the interfacial oxide layer. Intriguingly, a distinct and nonmonotonic exchange bias trend is observed as a function of temperature below 140 K. The occurrence of exchange bias induced by a "preset field" implies that the prevailing phase in the polycrystalline surface oxide is ferrimagnetic Fe 3 O 4 . Moreover, the exchange bias induced by the ferrimagnetic Fe 3 O 4 is significantly modulated by the presence of the van der Waals antiferromagnetic CrPS 4 layer, forming a heterostructure, along with additional iron oxide phases within the oxide layer. These findings underscore the intricate and complex nature of exchange bias in van der Waals heterostructures, highlighting their potential for tailored manipulation and control.

Altermagnetism represents an emergent collinear magnetic phase with compensated order and an unconventional alternating even-parity wave spin order in the non-relativistic band structure. We investigate directly this unconventional band splitting near the Fermi energy through spin-integrated soft X-ray angular resolved photoemission spectroscopy. The experimentally obtained angle-dependent photoemission intensity, acquired from epitaxial thin films of the predicted altermagnet CrSb, demonstrates robust agreement with the corresponding band structure calculations. In particular, we observe the distinctive splitting of an electronic band on a low-symmetry path in the Brilliouin zone that connects two points featuring symmetry-induced degeneracy. The measured large magnitude of the spin splitting of approximately 0.6 eV and the position of the band just below the Fermi energy underscores the significance of altermagnets for spintronics based on robust broken time reversal symmetry responses arising from exchange energy scales, akin to ferromagnets, while remaining insensitive to external magnetic fields and possessing THz dynamics, akin to antiferromagnets., (© 2024. The Author(s).)

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., Competing Interests: Conflict of Interest The authors declare no competing interests., (© The Author(s) 2024. Published by Oxford University Press on behalf of the Microscopy Society of America.)

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 (Tm 3 Fe 5 O 12 , 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.

Polymorphism (and its extended form - pseudopolymorphism) in solids is ubiquitous in mineralogy, crystallography, chemistry/biochemistry, materials science, and the pharmaceutical industries. Despite the difficulty of controlling (pseudo-)polymorphism, the realization of specific (pseudo-)polymorphic phases and associated boundary structures is an efficient route to enhance material performance for energy conversion and electromechanical applications. Here, this work applies the pseudopolymorphic phase (PP) concept to a thermoelectric copper sulfide, Cu 2- x S (x ≤ 0.25), via CuBr 2 doping. A peak ZT value of 1.25 is obtained at 773 K in Cu 1.8 S + 3 wt% CuBr 2 , which is 2.3 times higher than that of a pristine Cu 1.8 S sample. Atomic-resolution scanning transmission electron microscopy confirms the transformation of pristine Cu 1.8 S low digenite into PP-engineered high digenite, as well as the formation of (semi-)coherent interfaces between different PPs, which is expected to enhance phonon scattering. The results demonstrate that PP engineering is an effective approach for achieving improved thermoelectric performance in Cu-S compounds. It is also expected to be useful in other materials., (© 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.)

We have prepared ferromagnetic nanostructures intended for the investigation of high-frequency magnetization dynamics in permalloy (Py) nanodisks using Lorentz transmission electron microscopy (LTEM) and electron holography. Py nanodisks were fabricated on thin silicon nitride (SiN) membranes using three different fabrication methods: lift-off, ion beam etching (IBE), and stencil lithography. They were further analyzed using different instruments, including scanning electron microscopy, LTEM, and electron holography. A bilayer of positive PMMA resist was utilized in the first fabrication method to form an undercut structure that guarantees a clean lift-off procedure. The second approach used dry etching with an Ar beam to etch a thin Py film, while an electron-beam-patterned negative resist mask kept the desired structure. In the third process, nanostencils (shadow masks) with submicrometer apertures were milled on SiN membranes using a focused ion beam. Furthermore, we have developed a new TEM sample preparation method, where we fabricated Py nanostructures on a bulk substrate with a SiN buffer layer and etched the substrate to create a thin SiN membrane under the Py nanostructure. Finally, we observed the vortex dynamics of the Py nanodisk under magnetic fields using LTEM and off-axis electron holography. A correlation between preparation methods and the properties of the Py nanostructures was made., (Copyright © 2024, Williams et al.)

Dirac materials are characterized by the emergence of massless quasiparticles in their low-energy excitation spectrum that obey the Dirac Hamiltonian. Known examples of Dirac materials are topological insulators, d-wave superconductors, graphene, and Weyl and Dirac semimetals, representing a striking range of fundamental properties with potential disruptive applications. However, none of the Dirac materials identified so far shows metallic character. Here, we present evidence for the formation of free-standing molybdenene, a two-dimensional material composed of only Mo atoms. Using MoS 2 as a precursor, we induced electric-field-assisted molybdenene growth under microwave irradiation. We observe the formation of millimetre-long whiskers following screw-dislocation growth, consisting of weakly bonded molybdenene sheets, which, upon exfoliation, show metallic character, with an electrical conductivity of ~940 S m -1 . Molybdenene when hybridized with two-dimensional h-BN or MoS 2 , fetch tunable optical and electronic properties. As a proof of principle, we also demonstrate applications of molybdenene as a surface-enhanced Raman spectroscopy platform for molecular sensing, as a substrate for electron imaging and as a scanning probe microscope cantilever., (© 2023. The Author(s).)

Stray electric fields in free space generated by two biased gold needles have been quantified in comprehensive finite-element (FE) simulations, accompanied by first moment (FM) scanning TEM (STEM) and electron holography (EH) experiments. The projected electrostatic potential and electric field have been derived numerically under geometrical variations of the needle setup. In contrast to the FE simulation, application of an analytical model based on line charges yields a qualitative understanding. By experimentally probing the electric field employing FM STEM and EH under alike conditions, a discrepancy of about 60% became apparent initially. However, the EH setup suggests the reconstructed phase to be significantly affected by the perturbed reference wave effect, opposite to STEM where the field-free reference was recorded subsequently with unbiased needles in which possibly remaining electrostatic influences are regarded as being minor. In that respect, the observed discrepancy between FM imaging and EH is resolved after including the long-range potential landscape from FE simulations into the phase of the reference wave in EH., Competing Interests: Declaration of competing interest The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Knut Mueller–Caspary reports financial support was provided by Helmholtz Association of German Research Centres. Knut Mueller–Caspary reports financial support was provided by German Research Foundation. Jean Felix Dushimineza reports financial support was provided by Helmholtz Association of German Research Centres. Janghyun Jo reports financial support was provided by German Research Foundation., (Copyright © 2023 The Author(s). Published by Elsevier B.V. All rights reserved.)

Magnetic skyrmions and hopfions are topological solitons 1 -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. Skyrmions 2,3 are two-dimensional solitons resembling vortex-like string structures that can penetrate an entire sample. Hopfions 4-9 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 challenging 10 and has only been reported in a synthetic material 11 . 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., (© 2023. The Author(s).)

This work investigates the effect of copper substitution on the magnetic properties of SmCo 5 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 Co 3g sites not only stabilizes the formation of the SmCo 5 structure but also enhances magnetic anisotropy and coercivity. Density functional theory calculations indicate that Sm(Co 4 Cu 3g ) 5 possesses a higher single-ion anisotropy as compared to pure SmCo 5 . 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 SmCo 5 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.

Cryogenic electron microscopy can provide high-resolution reconstructions of macromolecules embedded in a thin layer of ice from which atomic models can be built de novo . However, the interaction between the ionizing electron beam and the sample results in beam-induced motion and image distortion, which limit the attainable resolutions. Sample charging is one contributing factor of beam-induced motions and image distortions, which is normally alleviated by including part of the supporting conducting film within the beam-exposed region. However, routine data collection schemes avoid strategies whereby the beam is not in contact with the supporting film, whose rationale is not fully understood. Here we characterize electrostatic charging of vitreous samples, both in imaging and in diffraction mode. We mitigate sample charging by depositing a single layer of conductive graphene on top of regular EM grids. We obtained high-resolution single-particle analysis (SPA) reconstructions at 2 Å when the electron beam only irradiates the middle of the hole on graphene-coated grids, using data collection schemes that previously failed to produce sub 3 Å reconstructions without the graphene layer. We also observe that the SPA data obtained with the graphene-coated grids exhibit a higher b factor and reduced particle movement compared to data obtained without the graphene layer. This mitigation of charging could have broad implications for various EM techniques, including SPA and cryotomography, and for the study of radiation damage and the development of future sample carriers. Furthermore, it may facilitate the exploration of more dose-efficient, scanning transmission EM based SPA techniques.

Magnetic nanoparticles can be functionalized in many ways for biomedical applications. Here, we combine four advantageous features in a novel Fe-Pt-Yb 2 O 3 core-shell nanoparticle. (a) The nanoparticles have a size of 10 nm allowing them to diffuse through neuronal tissue. (b) The particles are superparamagnetic after synthesis and ferromagnetic after annealing, enabling directional control by magnetic fields, enhance NMRI contrast, and hyperthermia treatment. (c) After neutron-activation of the shell, they carry low-energetic, short half-life β-radiation from 175 Yb, 177 Yb, and 177 Lu. (d) Additionally, the particles can be optically visualized by plasmonic excitation and luminescence. To demonstrate the potential of the particles for cancer treatment, we exposed cultured human glioblastoma cells (LN-18) to non-activated and activated particles to confirm that the particles are internalized, and that the β-radiation of the radioisotopes incorporated in the neutron-activated shell of the nanoparticles kills more than 98% of the LN-18 cancer cells, promising for future anti-cancer applications., Competing Interests: The authors declare no competing interests., (© 2023 The Author(s).)

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 ( H DL ) and field-like ( H FL ) effective fields in ultrathin Co films. We measure unexpectedly H FL / H DL 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 H FL , 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.

Characterisation of the electron beams trajectory in an electron microscope is possible in a few select commercial software packages, but these tools and their source code are not available in a free and accessible manner. This paper introduces the free and open-source software TEMGYM Advanced, which implements ray tracing methods that calculate the path of electrons through a magnetic or electrostatic lens and allow evaluation of the first-order properties and third-order geometric aberrations. Validation of the aberration coefficient calculations is performed by implementing two independent methods - the aberration integral and differential algebra (DA) methods and by comparing the results of each. This paper also demonstrates parallelised electron ray tracing through a series of magnetic components, which enables near real-time generation of a physically accurate beam-spot including aberrations and brings closer the realisation of a digital twin of an electron microscope. TEMGYM Advanced represents a valuable resource for the electron microscopy community, providing an accessible and open source means of characterising electron lenses. This software utilises the Python programming language to complement the growing ecosystem of free and open-source software within the electron microscopy community, and to facilitate the application of machine learning to an electron microscope digital twin for instrument automation. The software is available under GNU Public License number Three (GPL 3)., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 The Author(s). Published by Elsevier B.V. All rights reserved.)

An interactive simulation of a transmission electron microscope (TEM) called TEMGYM Basic is developed here, which enables users to understand how to operate and control an electron beam without the need to access an instrument. TEMGYM Basic allows users to familiarize themselves with alignment procedures offline, reducing the time and money required to become a proficient TEM operator. In addition to teaching the basics of electron beam alignments, the software enables users to create bespoke microscope configurations and develop an understanding of how to operate the configurations without sitting at a microscope. TEMGYM Basic also creates static ray diagram figures for a given lens configuration. The available components include apertures, lenses, quadrupoles, deflectors and biprisms. The software design uses first-order ray transfer matrices to calculate ray paths through each electron microscope component, and the program is developed entirely in Python to facilitate compatibility with machine-learning packages for future exploration of automated control., (© David Landers et al. 2023.)

Magnetoelasticity is the bond between magnetism and mechanics, but the intricate mechanisms via which magnetic states change due to mechanical strain remain poorly understood. Here, we provide direct nanoscale observations of how tensile strain modifies magnetic domains in a ferromagnetic Ni thin plate using in situ Fresnel defocus imaging, off-axis electron holography and a bimetallic deformation device. We present quantitative measurements of magnetic domain wall structure and its transformations as a function of strain. We observe the formation and dissociation of strain-induced periodic 180° magnetic domain walls perpendicular to the strain axis. The magnetization transformation exhibits stress-determined directional sensitivity and is reversible and tunable through the size of the nanostructure. In this work, we provide direct evidence for expressive and deterministic magnetic hardening in ferromagnetic nanostructures, while our experimental approach allows quantifiable local measurements of strain-induced changes in the magnetic states of nanomaterials., (© 2023. The Author(s).)

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., Competing Interests: Conflict of Interest The authors declare that they have no competing interest., (© The Author(s) 2023. Published by Oxford University Press on behalf of the Microscopy Society of America.)

A complete analysis including finite element method (FEM) calculation, focal length properties, and thirdorder geometric aberrations of the open-source electrostatic lens from the NanoMi project is presented. The analysis is carried out by the software TEMGYM Advanced, a free package developed to carry out ray-tracing and lens characterisation in Python. Previously TEMGYM Advanced has shown how to analyse the aberrations of analytical lens fields; this paper expands upon this work to demonstrate how to apply a suitable fitting method to discrete lens fields obtained via FEM methods so that the aberrations of real lens designs can be calculated. Each software platform used in this paper is freely available in the community and creates a free and viable alternative to commercial lens design packages., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023. Published by Elsevier Ltd.)

Topological spin textures are of great interest for both fundamental physics and applications in spintronics. The Dzyaloshinskii-Moriya interaction underpins the formation of single-twisted magnetic solitons or multi-twisted magnetic skyrmions in magnetic materials with different crystallographic symmetries. However, topological transitions between these two kinds of topological objects have not been verified experimentally. Here, the direct observation of transformations from a chiral soliton lattice (CSL) to magnetic skyrmions in a nanostripe of the monoaxial chiral magnet CrNb 3 S 6  using Lorentz transmission electron microscopy is reported. In the presence of an external magnetic field, helical spin structures first transform into CSLs and then evolve into isolated elongated magnetic skyrmions. The detailed spin textures of the elongated magnetic skyrmions are resolved using off-axis electron holography and are shown to comprise two merons, which enclose their ends and have unit total topological charge. Magnetic dipolar interactions are shown to play a key role in the magnetic soliton-skyrmion transformation, which depends sensitively on nanostripe width. The findings here, which are consistent with micromagnetic simulations, enrich the family of topological magnetic states and their transitions and promise to further stimulate the exploration of their emergent electromagnetic properties., (© 2023 Wiley-VCH GmbH.)

The key to optimizing spatial resolution in a state-of-the-art scanning transmission electron microscope is the ability to measure and correct for electron optical aberrations of the probe-forming lenses precisely. Several diagnostic methods for aberration measurement and correction have been proposed, albeit often at the cost of relatively long acquisition times. Here, we illustrate how artificial intelligence can be used to provide near-real-time diagnosis of aberrations from individual Ronchigrams. The demonstrated speed of aberration measurement is important because microscope conditions can change rapidly. It is also important for the operation of MEMS-based hardware correction elements, which have less intrinsic stability than conventional electromagnetic lenses., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper. The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Vincenzo Grillo reports financial support was provided by Horizon 2020. Rafal E. Dunin-Borkowski reports financial support was provided by Horizon 2020., (Copyright © 2022 The Authors. Published by Elsevier B.V. All rights reserved.)

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.

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 Ce 0.9 Gd 0.1 O 2-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 H 2 O, CH 4 , H 2 , CO 2 and H 2 S. Furthermore, our approach is highly scalable and applicable to a wide variety of ion conducting thin layers, including Y 0.08 Zr 0.92 O 2-δ , Ce 0.9 Sm 0.1 O 2-δ and Ce 0.9 Pr 0.1 O 2-δ ., (© 2022 Wiley-VCH GmbH.)

With the ever-increasing use of Li-ion batteries, especially due to their adoption in electric vehicles, their safety is in prime focus. Thus, the all-solid-state batteries (ASSBs) that use solid electrolytes instead of liquid electrolytes, which reduce the risk of flammability, have been the center stage of battery research for the last few years. However, in the ASSB, the ion transportation through the solid-solid electrolyte-electrode interface poses a challenge due to contact and chemical/electrochemical stability issues. Applying a suitable coating around the electrode and/or electrolyte particles offers a convenient solution, leading to better performance. For this, researchers are screening potential electronic/ionic conductive and nonconductive coatings to find the best coatings with suitable thickness for long-term chemical, electrochemical, and mechanical stability. Operando transmission electron microscopy (TEM) couples high spatial resolution with high temporal resolution to allow visualization of dynamic processes, and thus is an ideal tool to evaluate electrode/electrolyte coatings via studying (de)lithiation at a single particle level in real-time. However, the accumulated electron dose during a typical high-resolution in situ work may affect the electrochemical pathways, evaluation of which can be time-consuming. The current protocol presents an alternative procedure in which the potential coatings are applied on Si nanoparticles and are subjected to (de)lithiation during operando TEM experiments. The high volume changes of Si nanoparticles during (de)lithiation allow monitoring of the coating behavior at a relatively low magnification. Thus, the whole process is very electron-dose efficient and offers quick screening of potential coatings.

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 H 2 can be extracted from methanol with high performance. Here, we present noble-metal-free Cu-WC/W plasmonic nanohybrids which exhibit unsurpassed solar H 2 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 CH 3 OH plasmonic reforming with C 3 -dominated liquid products and 100% selective gaseous H 2 . Such high efficiency, without any CO x emission, can be sustained for over a thousand-hour operation without obvious degradation.

Electrostatic charging of specimens during electron, photon or ion irradiation is a complicated and poorly understood phenomenon, which can affect the acquisition and interpretation of experimental data and alter the functional properties of the constituent materials. It is usually linked to secondary electron emission, but also depends on the geometry and electrical properties of the specimen. Here, we use off-axis electron holography in the transmission electron microscope to study electron-beam-induced charging of an insulating Al 2 O 3 nanotip on a conducting support. The measurements are performed under parallel electron illumination conditions as a function of specimen temperature, electron dose, primary electron energy and surface cleanliness. We observe a lack of reproducibility of charge density measurements after cycling the specimen temperature. Surprisingly, we find both positively and negatively charged regions in closely adjacent parts of the specimen., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 The Author(s). Published by Elsevier B.V. All rights reserved.)

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 F 2+ centers induced by oxygen vacancies at the MgO nanocube surfaces.

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.

Recently proposed bimetallic octahedral Pt-Ni electrocatalysts for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cell (PEMFC) cathodes suffer from particle instabilities in the form of Ni corrosion and shape degradation. Advanced trimetallic Pt-based electrocatalysts have contributed to their catalytic performance and stability. In this work, we propose and analyse a novel quaternary octahedral (oh-)Pt nanoalloy concept with two distinct metals serving as stabilizing surface dopants. An efficient solvothermal one-pot strategy was developed for the preparation of shape-controlled oh-PtNi catalysts doped with Rh and Mo in its surface. The as-prepared quaternary octahedral PtNi(RhMo) catalysts showed exceptionally high ORR performance accompanied by improved activity and shape integrity after stability tests compared to previously reported bi- and tri-metallic systems. Synthesis, performance characteristics and degradation behaviour are investigated targeting deeper understanding for catalyst system improvement strategies. A number of different operando and on-line analysis techniques were employed to monitor the structural and elemental evolution, including identical location scanning transmission electron microscopy and energy dispersive X-ray analysis (IL-STEM-EDX), operando wide angle X-ray spectroscopy (WAXS), and on-line scanning flow cell inductively coupled plasma mass spectrometry (SFC-ICP-MS). Our studies show that doping PtNi octahedral catalysts with small amounts of Rh and Mo suppresses detrimental Pt diffusion and thus offers an attractive new family of shaped Pt alloy catalysts for deployment in PEMFC cathode layers., Competing Interests: There are no conflicts to declare., (This journal is © The Royal Society of Chemistry.)

Inline holography in the transmission electron microscope is a versatile technique which provides real-space phase information that can be used for the correction of imaging aberrations, as well as for measuring electric and magnetic fields and strain distributions. It is able to recover high-spatial-frequency contributions of the phase effectively but suffers from the weak transfer of low-spatial-frequency information, as well as from incoherent scattering. Here, we combine gradient flipping and phase prediction in an iterative flux-preserving focal series reconstruction algorithm with incoherent background subtraction that gives extensive access to the missing low spatial frequencies. A procedure for optimizing the reconstruction parameters is presented, and results from Fe-filled C nanospheres, and MgO cubes are compared with phase images obtained using off-axis holography., (© 2022. The Author(s).)

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.

Over the past decade, advances in the colloidal syntheses of octahedral-shaped Pt-Ni alloy nanocatalysts for use in fuel cell cathodes have raised our atomic-scale control of particle morphology and surface composition, which, in turn, helped raise their catalytic activity far above that of benchmark Pt catalysts. Future fuel cell deployment in heavy-duty vehicles caused the scientific priorities to shift from alloy particle activity to stability. Larger particles generally offer enhanced thermodynamic stability, yet synthetic approaches toward larger octahedral Pt-Ni alloy nanoparticles have remained elusive. In this study, we show how a simple manipulation of solvothermal synthesis reaction kinetics involving depressurization of the gas phase at different stages of the reaction allows tuning the size of the resulting octahedral nanocatalysts to previously unachieved scales. We then link the underlying mechanism of our approach to the classical "LaMer" model of nucleation and growth. We focus on large, annealed Mo-doped Pt-Ni octahedra and investigate their synthesis, post-synthesis treatments, and elemental distribution using advanced electron microscopy. We evaluate the electrocatalytic ORR performance and stability and succeed to obtain a deeper understanding of the enhanced stability of a new class of relatively large, active, and long-lived Mo-doped Pt-Ni octahedral catalysts for the cathode of PEMFCs.

We investigate potential improvements in using electron cryomicroscopy to image thick specimens with high-resolution phase contrast imaging. In particular, using model experiments, electron scattering theory, Monte Carlo and multislice simulations, we determine the potential for improving electron cryomicrographs of proteins within a cell using chromatic aberration (C c ) correction. We show that inelastically scattered electrons lose a quantifiable amount of spatial coherence as they transit the specimen, yet can be used to enhance the signal from thick biological specimens (in the 1000 to 5000 Å range) provided they are imaged close to focus with an achromatic lens. This loss of information quantified here, which we call "specimen induced decoherence", is a fundamental limit on imaging biological molecules in situ. We further show that with foreseeable advances in transmission electron microscope technology, it should be possible to directly locate and uniquely identify sub-100 kDa proteins without the need for labels, in a vitrified specimen taken from a cell., (Copyright © 2022 MRC Laboratory of Molecular Biology. Published by Elsevier B.V. All rights reserved.)

Two-dimensional (2D) van der Waals magnets have drawn considerable attention in recent years triggered by the huge interest in novel magnetism and spintronic devices. Magnetic measurement of 2D van der Waals (vdW) magnets is crucial to understand the physical origin of magnetism in 2D limits. Therefore, advanced magnetic characterization techniques are highly required. However, only a limited number of such techniques are available due to the extremely small volume of 2D vdW magnets. Here, we introduce the electron magnetic chiral dichroism (EMCD) technique in transmission electron microscope (TEM) to measure 2D vdW crystals. In comparison with some other already-employed techniques in 2D magnets, EMCD is able to quantitatively measure magnetic parameters in three orthogonal directions at nanometer or even at atomic scale. We then perform EMCD simulations on several typical 2D vdW magnets with respect to the accelerating voltage, the number of atomic layers and beam tilt under zone axial orientation. The intensity and distribution of EMCD signals in three orthogonal directions are given in the diffraction plane, thereby providing an optimized design to achieve EMCD measurements. Finally, we discuss the signal-to-noise-ratio and required electron dose in order to obtain a measurable EMCD signal for 2D vdW magnets. Our results provide a feasibility analysis and guideline to measure 2D vdW magnets in future experiments., (Copyright © 2022 The Authors. Published by Elsevier B.V. All rights reserved.)

Magnetic high-entropy alloys (HEAs) are a new category of high-performance magnetic materials, with multicomponent concentrated compositions and complex multi-phase structures. Although there have been numerous reports of their interesting magnetic properties, there is very limited understanding about the interplay between their hierarchical multi-phase structures and the resulting magnetic behavior. We reveal for the first time the influence of a hierarchically decomposed B2 + A2 structure in an AlCo 0.5 Cr 0.5 FeNi HEA on the formation of magnetic vortex states within individual A2 (disordered BCC) precipitates, which are distributed in an ordered B2 matrix that is weakly ferromagnetic. Non-magnetic or weakly ferromagnetic B2 precipitates in large magnetic domains of the A2 phase, and strongly magnetic Fe-Co-rich interphase A2 regions, are also observed. These results provide important insight into the origin of coercivity in this HEA, which can be attributed to a complex magnetization process that includes the successive reversal of magnetic vortices., Competing Interests: The authors declare no competing interests., (© 2022 The Authors.)

Conformal coating of silicon (Si) anode particles is a common strategy for improving their mechanical integrity, to mitigate battery capacity fading due to particle volume expansion, which can result in particle crumbling due to lithiation induced strain and excessive solid-electrolyte interface formation. Here, we use operando transmission electron microscopy in an open cell to show that TiO 2 coatings on Si/SiO 2 particles undergo thickness dependent rupture on battery cycling where thicker coatings crumble more readily than thinner (∼5 nm) coatings, which corroborates the difference in their capacities.

Magnetic skyrmions are stable topological solitons with complex non-coplanar spin structures. Their nanoscopic size and the low electric currents required to control their motion has opened a new field of research, skyrmionics, that aims for the usage of skyrmions as information carriers. Further advances in skyrmionics call for a thorough understanding of their three-dimensional (3D) spin texture, skyrmion-skyrmion interactions and the coupling to surfaces and interfaces, which crucially affect skyrmion stability and mobility. Here, we quantitatively reconstruct the 3D magnetic texture of Bloch skyrmions with sub-10-nanometre resolution using holographic vector-field electron tomography. The reconstructed textures reveal local deviations from a homogeneous Bloch character within the skyrmion tubes, details of the collapse of the skyrmion texture at surfaces and a correlated modulation of the skyrmion tubes in FeGe along their tube axes. Additionally, we confirm the fundamental principles of skyrmion formation through an evaluation of the 3D magnetic energy density across these magnetic solitons., (© 2021. The Author(s).)

The shuttling behavior and sluggish conversion kinetics of the intermediate lithium polysulfides (LiPS) represent the main obstructions to the practical application of lithium-sulfur batteries (LSBs). Herein, a 1D π-d conjugated metal-organic framework (MOF), Ni-MOF-1D, is presented as an efficient sulfur host to overcome these limitations. Experimental results and density functional theory calculations demonstrate that Ni-MOF-1D is characterized by a remarkable binding strength for trapping soluble LiPS species. Ni-MOF-1D also acts as an effective catalyst for S reduction during the discharge process and Li 2 S oxidation during the charging process. In addition, the delocalization of electrons in the π-d system of Ni-MOF-1D provides a superior electrical conductivity to improve electron transfer. Thus, cathodes based on Ni-MOF-1D enable LSBs with excellent performance, for example, impressive cycling stability with over 82% capacity retention over 1000 cycles at 3 C, superior rate performance of 575 mAh g -1 at 8 C, and a high areal capacity of 6.63 mAh cm -2 under raised sulfur loading of 6.7 mg cm -2 . The strategies and advantages here demonstrated can be extended to a broader range of π-d conjugated MOFs materials, which the authors believe have a high potential as sulfur hosts in LSBs., (© 2022 Wiley-VCH GmbH.)

Progress towards analysing transitions between steady states demands improvements in time-resolved imaging, both for fundamental research and for applications in information technology. Transmission electron microscopy is a powerful technique for investigating the atomic structure, chemical composition and electromagnetic properties of materials with high spatial resolution and precision. However, the extraction of information about dynamic processes in the ps time regime is often not possible without extensive modification to the instrument while requiring careful control of the operation conditions to not compromise the beam quality. Here, we avoid these drawbacks by combining a delay line detector with continuous illumination in a transmission electron microscope. We visualize the gyration of a magnetic vortex core in real space and show that magnetization dynamics up to frequencies of 2.3 GHz can be resolved with down to ∼122ps temporal resolution by studying the interaction of an electron beam with a microwave magnetic field. In the future, this approach promises to provide access to resonant dynamics by combining high spatial resolution with sub-ns temporal resolution., (Copyright © 2021 The Authors. Published by Elsevier B.V. All rights reserved.)

Using a combination of in situ bulk and surface characterization techniques, we provide atomic-scale insight into the complex surface and bulk dynamics of a LaNiO 3 perovskite material during heating in vacuo . Driven by the outstanding activity LaNiO 3 in the methane dry reforming reaction (DRM), attributable to the decomposition of LaNiO 3 during DRM operation into a Ni//La 2 O 3 composite, we reveal the Ni exsolution dynamics both on a local and global scale by in situ electron microscopy, in situ X-ray diffraction and in situ X-ray photoelectron spectroscopy. To reduce the complexity and disentangle thermal from self-activation and reaction-induced effects, we embarked on a heating experiment in vacuo under comparable experimental conditions in all methods. Associated with the Ni exsolution, the remaining perovskite grains suffer a drastic shrinkage of the grain volume and compression of the structure. Ni particles mainly evolve at grain boundaries and stacking faults. Sophisticated structure analysis of the elemental composition by electron-energy loss mapping allows us to disentangle the distribution of the different structures resulting from LaNiO 3 decomposition on a local scale. Important for explaining the DRM activity, our results indicate that most of the Ni moieties are oxidized and that the formation of NiO occurs preferentially at grain edges, resulting from the reaction of the exsolved Ni particles with oxygen released from the perovskite lattice during decomposition via a spillover process from the perovskite to the Ni particles. Correlating electron microscopy and X-ray diffraction data allows us to establish a sequential two-step process in the decomposition of LaNiO 3 via a Ruddlesden-Popper La 2 NiO 4 intermediate structure. Exemplified for the archetypical LaNiO 3 perovskite material, our results underscore the importance of focusing on both surface and bulk characterization for a thorough understanding of the catalyst dynamics and set the stage for a generalized concept in the understanding of state-of-the art catalyst materials on an atomic level., Competing Interests: The authors declare no competing financial interest., (© 2021 The Authors. Published by American Chemical Society.)

Benefitting from exceptional energy storage performance, dielectric-based capacitors are playing increasingly important roles in advanced electronics and high-power electrical systems. Nevertheless, a series of unresolved structural puzzles represent obstacles to further improving the energy storage performance. Compared with ferroelectrics and linear dielectrics, antiferroelectric materials have unique advantages in unlocking these puzzles due to the inherent coupling of structural transitions with the energy storage process. In this review, we summarize the most recent studies about in-situ structural phase transitions in PbZrO 3 -based and NaNbO 3 -based systems. In the context of the ultrahigh energy storage density of SrTiO 3 -based capacitors, we highlight the necessity of extending the concept of antiferroelectric-to-ferroelectric (AFE-to-FE) transition to broader antiferrodistortive-to-ferrodistortive (AFD-to-FD) transition for materials that are simultaneously ferroelastic. Combining discussion of the factors driving ferroelectricity, electric-field-driven metal-to-insulator transition in a (La 1-x Sr x )MnO 3 electrode is emphasized to determine the role of ionic migration in improving the storage performance. We believe that this review, aiming at depicting a clearer structure-property relationship, will be of benefit for researchers who wish to carry out cutting-edge structure and energy storage exploration.

Electron beam shaping by sculpted thin films relies on electron-matter interactions and the wave nature of electrons. It can be used to study physical phenomena of special electron beams and to develop technological applications in electron microscopy that offer new and improved measurement techniques and increased resolution in different imaging modes. In this Perspective, we review recent applications of sculpted thin films for electron orbital angular momentum sorting, improvements in phase contrast transmission electron microscopy, and aberration correction. For the latter, we also present new results of our work toward correction of the spherical aberration of Lorentz scanning transmission electron microscopes and suggest a method to correct chromatic aberration using thin films. This review provides practical insight for researchers in the field and motivates future progress in electron microscopy., Competing Interests: The authors declare no competing financial interest., (© 2021 The Authors. Published by American Chemical Society.)