Statistically elucidated responses from low-signal contrast mechanisms in ultrafast electron microscopy.

The emergence of ultrafast electron microscopy (UEM) has enabled the discovery of strongly correlated dynamic mechanisms, including electron-phonon coupling, structural phase transitions, thermal transport, and electromagnetic deflection. Most UEM systems operate stroboscopically, meaning that the technique is susceptible to artifacts, mistakes, and misinterpretation of the data due to extensive experimental effort. In contrast to the ultrafast designation, data acquisition is extraordinarily slow because the electron beam has significantly reduced signal compared to traditional transmission electron microscopy due to pulsing the electron beam.

Sub-unit-cell-segmented ferroelectricity in brownmillerite oxides by phonon decoupling.

The ultimate scaling limit in ferroelectric switching has been attracting broad attention in the fields of materials science and nanoelectronics. Despite immense efforts to scale down ferroelectric features, however, only few materials have been shown to exhibit ferroelectricity at the unit-cell level. Here we report a controllable unit-cell-scale domain in brownmillerite oxides consisting of alternating octahedral/tetrahedral layers.

Charge Density Wave and Ferromagnetism in Intercalated CrSBr.

In materials with 1D electronic bands, electron-electron interactions can produce intriguing quantum phenomena, including spin-charge separation and charge density waves (CDW). Most of these systems, however, are non-magnetic, motivating a search for anisotropic materials where the coupling of charge and spin may affect emergent quantum states. Here, chemical intercalation of the van der Waals magnetic semiconductor CrSBr yields Li(tetrahydrofuran)CrSBr, which possesses an electronically driven quasi-1D CDW with an onset temperature above room temperature.

Single-Layer Magnet Phase in Intrinsic Magnetic Topological Insulators, [MnTe][BiTe], Far beyond the Thermodynamic Limit.

The intrinsic magnetic topological insulator (IMTI) family [MnTe][BiTe] has demonstrated magneto-topological properties dependent on , making it a promising platform for advanced electronics and spintronics. However, due to technical barriers in sample synthesis, their properties in the large limit remain unknown. To overcome this, we utilized the atomic layer-by-layer molecular beam epitaxy (ALL-MBE) technique and achieved IMTIs with as large as 15, far beyond that previously reported in bulk crystals or thin films.

Electric Field Control of Magnetic Skyrmion Helicity in a Centrosymmetric 2D van der Waals Magnet.

Two-dimensional van der Waals magnets hosting topological magnetic textures, such as skyrmions, show promise for spintronics and quantum computing. Electrical control of these topological spin textures is crucial for enhancing operational performance and functionality. Here, using electron microscopy combined with electric and magnetic biasing, we show that the skyrmion helicity in insulating CrGeTe can be controlled by the direction of the external electric field applied during the field cooling process.

Correlated spin-wave generation and domain-wall oscillation in a topologically textured magnetic film.

Spin waves, or magnons, are essential for next-generation energy-efficient spintronics and magnonics. Yet, visualizing spin-wave dynamics at nanoscale and microwave frequencies remains a formidable challenge due to the lack of spin-sensitive, time-resolved microscopy. Here we report a breakthrough in imaging dipole-exchange spin waves in a ferromagnetic film owing to the development of laser-free ultrafast Lorentz electron microscopy, which is equipped with a microwave-mediated electron pulser for high spatiotemporal resolution.

Atomic resolution scanning transmission electron microscopy at liquid helium temperatures for quantum materials.

Fundamental quantum phenomena in condensed matter, ranging from correlated electron systems to quantum information processors, manifest their emergent characteristics and behaviors predominantly at low temperatures. This necessitates the use of liquid helium (LHe) cooling for experimental observation. Atomic resolution scanning transmission electron microscopy combined with LHe cooling (cryo-STEM) provides a powerful characterization technique to probe local atomic structural modulations and their coupling with charge, spin and orbital degrees-of-freedom in quantum materials.

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The exploration of 1D magnetism, frequently portrayed as spin chains, constitutes an actively pursued research field that illuminates fundamental principles in many-body problems and applications in magnonics and spintronics. The inherent reduction in dimensionality often leads to robust spin fluctuations, impacting magnetic ordering and resulting in novel magnetic phenomena. Here, structural, magnetic, and optical properties of highly anisotropic 2D van der Waals antiferromagnets that uniquely host spin chains are explored.

Effect of Surface Oxidation and Crystal Thickness on the Magnetic Properties and Magnetic Domain Structures of CrGeTe.

van der Waals (vdW) magnetic materials, such as CrGeTe (CGT), show promise for memory and logic applications. This is due to their broadly tunable magnetic properties and the presence of topological magnetic features such as skyrmionic bubbles. A systematic study of thickness and oxidation effects on magnetic domain structures is important for designing devices and vdW heterostructures for practical applications.

Emergent layer stacking arrangements in c-axis confined MoTe.

The layer stacking order in 2D materials strongly affects functional properties and holds promise for next-generation electronic devices. In bulk, octahedral MoTe possesses two stacking arrangements, the ferroelectric Weyl semimetal T phase and the higher-order topological insulator 1T' phase. However, in thin flakes of MoTe, it is unclear if the layer stacking follows the T, 1T', or an alternative stacking sequence.

Hysteretic Responses of Skyrmion Lattices to Electric Fields in Magnetoelectric CuOSeO.

Electric field control of topologically nontrivial magnetic textures, such as skyrmions, provides a paradigm shift for future spintronics beyond the current silicon-based technology. While significant progress has been made by X-ray and neutron scattering studies, direct observation of such nanoscale spin structures and their dynamics driven by external electric fields remains a challenge in understanding the underlying mechanisms and harness functionalities. Here, using Lorentz transmission electron microscopy combined with electric and magnetic fields at liquid helium temperatures, we report the crystallographic orientation-dependent skyrmion responses to electric fields in thin slabs of magnetoelectric CuOSeO.

Toward accurate measurement of electromagnetic field by retrieving and refining the center position of non-uniform diffraction disks in Lorentz 4D-STEM.

Recent advancement in scanning transmission electron microscopy (STEM) allows the use of 4D-STEM, a technique that captures an electron diffraction pattern at each scan point in STEM, to measure electrostatic and magnetic potential and field in materials. However, accurate measurement, separation of the magnetic and electric signals, and removal of artifacts remain challenging, especially in the presence of complex non-uniform diffraction contrast within the disks. Here, based on dynamic simulations of 4D-STEM patterns built upon superstructures consisting of millions of atoms to account for different sample thickness and edge geometries, we show how the shape and intensity distribution of the central disk are affected by multiple scattering.

Characterization of transverse electron pulse trains using RF powered traveling wave metallic comb striplines.

Advancements in ultrafast electron microscopy have allowed elucidation of spatially selective structural dynamics. However, as the spatial resolution and imaging capabilities have made progress, quantitative characterization of the electron pulse trains has not been reported at the same rate. In fact, inexperienced users have difficulty replicating the technique because only a few dedicated microscopes have been characterized thoroughly.

Topological Hall Effect Anisotropy in Kagome Bilayer Metal Fe_{3}Sn_{2}.

Kagome lattice materials have attracted growing interest for their topological properties and flatbands in electronic structure. We present a comprehensive study on the anisotropy and out-of-plane electric transport in Fe_{3}Sn_{2}, a metal with bilayer of Fe kagome planes and with massive Dirac fermions that features high-temperature noncollinear magnetic structure and magnetic skyrmions. For the electrical current path along the c axis, in micron-size crystals, we found a large topological Hall effect over a wide temperature range down to spin-glass state.

Superconducting Fourfold Fe(Te,Se) Film on Sixfold Magnetic MnTe via Hybrid Symmetry Epitaxy.

Epitaxial Fe(Te,Se) thin films have been grown on various substrates but never been grown on magnetic layers. Here we report the epitaxial growth of fourfold Fe(Te,Se) film on a sixfold antiferromagnetic insulator, MnTe. The Fe(Te,Se)/MnTe heterostructure shows a clear superconducting transition at around 11 K, and the critical magnetic field measurement suggests the origin of the superconductivity to be bulk-like.

Coupling between magnetic order and charge transport in a two-dimensional magnetic semiconductor.

Semiconductors, featuring tunable electrical transport, and magnets, featuring tunable spin configurations, form the basis of many information technologies. A long-standing challenge has been to realize materials that integrate and connect these two distinct properties. Two-dimensional (2D) materials offer a platform to realize this concept, but known 2D magnetic semiconductors are electrically insulating in their magnetic phase.

Stroboscopic ultrafast imaging using RF strip-lines in a commercial transmission electron microscope.

The development of ultrafast electron microscopy (UEM), specifically stroboscopic imaging, has brought the study of structural dynamics to a new level by overcoming the spatial limitations of ultrafast spectroscopy and the temporal restrictions of traditional TEM simultaneously. Combining the concepts governing both techniques has enabled direct visualization of dynamics with spatiotemporal resolutions in the picosecond-nanometer regime. Here, we push the limits of imaging using a pulsed electron beam via RF induced transverse deflection based on the newly developed 200 keV frequency-tunable strip-line pulser.

Topological spin/structure couplings in layered chiral magnet CrTaS: The discovery of spiral magnetic superstructure.

Chiral magnets have recently emerged as hosts for topological spin textures and related transport phenomena, which can find use in next-generation spintronic devices. The coupling between structural chirality and noncollinear magnetism is crucial for the stabilization of complex spin structures such as magnetic skyrmions. Most studies have been focused on the physical properties in homochiral states favored by crystal growth and the absence of long-ranged interactions between domains of opposite chirality.

Hybrid Symmetry Epitaxy of the Superconducting Fe(Te,Se) Film on a Topological Insulator.

It is challenging to grow an epitaxial 4-fold compound superconductor (SC) on a 6-fold topological insulator (TI) platform due to the stringent lattice-matching requirement. Here, we demonstrate that Fe(Te,Se) can grow epitaxially on a TI (BiTe) layer due to accidental, uniaxial lattice match, which is dubbed as "hybrid symmetry epitaxy". This new growth mode is critical to stabilizing robust superconductivity with as high as 13 K.

Spacer-Layer-Tunable Magnetism and High-Field Topological Hall Effect in Topological Insulator Heterostructures.

Controlling magnetic order in magnetic topological insulators (MTIs) is a key to developing spintronic applications with MTIs and is commonly achieved by changing the magnetic doping concentration, which inevitably affects the spin-orbit coupling strength and the topological properties. Here, we demonstrate tunable magnetic properties in topological heterostructures over a wide range, from a ferromagnetic phase with a Curie temperature of around 100 K all the way to a paramagnetic phase, while keeping the overall chemical composition the same, by controlling the thickness of nonmagnetic spacer layers between two atomically thin magnetic layers. This work showcases that spacer-layer control is a powerful tool to manipulate magneto-topological functionalities in MTI heterostructures.

Strain-Induced Atomic-Scale Building Blocks for Ferromagnetism in Epitaxial LaCoO.

The origin of strain-induced ferromagnetism, which is robust regardless of the type and degree of strain in LaCoO (LCO) thin films, is enigmatic despite intensive research efforts over the past decade. Here, by combining scanning transmission electron microscopy with density functional theory calculations, we report that the ferromagnetism does not emerge directly from the strain itself but rather from the creation of compressed structural units within ferroelastically formed twin-wall domains. The compressed structural units are magnetically active with the rocksalt-type high-spin/low-spin order.

characterization of conductive filaments during resistive switching in Mott VO.

Vanadium dioxide (VO) has attracted much attention owing to its metal-insulator transition near room temperature and the ability to induce volatile resistive switching, a key feature for developing novel hardware for neuromorphic computing. Despite this interest, the mechanisms for nonvolatile switching functioning as synapse in this oxide remain not understood. In this work, we use in situ transmission electron microscopy, electrical transport measurements, and numerical simulations on Au/VO/Ge vertical devices to study the electroforming process.