Topological Spin Textures in an Insulating van der Waals Ferromagnet.

Generation and control of topological spin textures constitutes one of the most exciting challenges of modern spintronics given their potential applications in information storage technologies. Of particular interest are magnetic insulators, which due to low damping, absence of Joule heating and reduced dissipation can provide energy-efficient spin-textures platform. Here, it is demonstrated that the interplay between sample thickness, external magnetic fields, and optical excitations can generate a prolific paramount of spin textures, and their coexistence in insulating CrBr3 van der Waals (vdW) ferromagnets. Using high-resolution magnetic force microscopy and large-scale micromagnetic simulation methods, the existence of a large region in T-B phase diagram is demonstrated where different stripe domains, skyrmion crystals, and magnetic domains exist and can be intrinsically selected or transformed to each-other via a phase-switch mechanism. Lorentz transmission electron microscopy unveils the mixed chirality of the magnetic textures that are of Bloch-type at given conditions but can be further manipulated into Néel-type or hybrid-type via thickness-engineering. The topological phase transformation between the different magnetic objects can be further inspected by standard photoluminescence optical probes resolved by circular polarization indicative of an existence of exciton-skyrmion coupling mechanism. The findings identify vdW magnetic insulators as a promising framework of materials for the manipulation and generation of highly ordered skyrmion lattices relevant for device integration at the atomic level.

Understanding the Effect of Curvature on the Magnetization Reversal of Three-Dimensional Nanohelices.

Comprehending the interaction between geometry and magnetism in three-dimensional (3D) nanostructures is important to understand the fundamental physics of domain wall (DW) formation and pinning. Here, we use focused-electron-beam-induced deposition to fabricate magnetic nanohelices with increasing helical curvature with height. Using electron tomography and Lorentz transmission electron microscopy, we reconstruct the 3D structure and magnetization of the nanohelices. The surface curvature, helical curvature, and torsion of the nanohelices are then quantified from the tomographic reconstructions. Furthermore, by using the experimental 3D reconstructions as inputs for micromagnetic simulations, we can reveal the influence of surface and helical curvature on the magnetic reversal mechanism. Hence, we can directly correlate the magnetic behavior of a 3D nanohelix to its experimental structure. These results demonstrate how the control of geometry in nanohelices can be utilized in the stabilization of DWs and control of the response of the nanostructure to applied magnetic fields.

Writing and Detecting Topological Charges in Exfoliated Fe5-xGeTe2.

Fe5-xGeTe2 is a promising two-dimensional (2D) van der Waals (vdW) magnet for practical applications, given its magnetic properties. These include Curie temperatures above room temperature, and topological spin textures─TST (both merons and skyrmions), responsible for a pronounced anomalous Hall effect (AHE) and its topological counterpart (THE), which can be harvested for spintronics. Here, we show that both the AHE and THE can be amplified considerably by just adjusting the thickness of exfoliated Fe5-xGeTe2, with THE becoming observable even in zero magnetic field due to a field-induced unbalance in topological charges. Using a complementary suite of techniques, including electronic transport, Lorentz transmission electron microscopy, and micromagnetic simulations, we reveal the emergence of substantial coercive fields upon exfoliation, which are absent in the bulk, implying thickness-dependent magnetic interactions that affect the TST. We detected a "magic" thickness t ≈ 30 nm where the formation of TST is maximized, inducing large magnitudes for the topological charge density (∼6.45 × 1020 cm-2), and the concomitant anomalous (ρxyA,max ≃22.6 µΩ cm) and topological (ρxyu,T 1≃5 µΩ cm) Hall resistivities at T ≈ 120 K. These values for ρxyA,max and ρxyu,T are higher than those found in magnetic topological insulators and, so far, the largest reported for 2D magnets. The hitherto unobserved THE under zero magnetic field could provide a platform for the writing and electrical detection of TST aiming at energy-efficient devices based on vdW ferromagnets.

Direct observation of magnetic ordering induced via systematic lattice disorder in artificial rhombus spin ices.

It is critical to understand the effect of lattice geometry on the order parameter of a condensed matter system, as it controls phase transitions in such systems. Artificial spin ices (ASIs) are two-dimensional lattices of Ising-like nanomagnets that provide an opportunity to explore such phenomena by lithographically controlling the lattice geometry to observe its influence on magnetic ordering and frustration effects. Here we report a systematic approach to studying the effects of disorder in rhombus ASIs generated from combinations of five vertex motifs. We investigate four geometries characterized by a geometric order parameter, with symmetries ranging from periodic to quasiperiodic to random. Lorentz transmission electron microscopy data indicates magnetic domain behavior depends on chains of strongly-coupled islands in the periodic and sixfold-twinned lattices, while the behavior of the disordered lattice is dominated by vertex motifs with large configurational degeneracy. Utilizing micromagnetic simulations, a quantitative analysis of the lattice energetics showed that the experimental rotationally-demagnetized state of the disordered ASI was closer in energy to the idealized ground state compared to other periodic and twinned ASIs. Our work provides a unique pathway for using degeneracy, magnetic frustration, and order to control the magnetization behavior of designer disordered systems.

Coexistence of Merons with Skyrmions in the Centrosymmetric Van Der Waals Ferromagnet Fe5- x GeTe2.

Fe5- x GeTe2 is a centrosymmetric, layered van der Waals (vdW) ferromagnet that displays Curie temperatures Tc (270-330 K) that are within the useful range for spintronic applications. However, little is known about the interplay between its topological spin textures (e.g., merons, skyrmions) with technologically relevant transport properties such as the topological Hall effect (THE) or topological thermal transport. Here, via high-resolution Lorentz transmission electron microscopy, it is shown that merons and anti-meron pairs coexist with Néel skyrmions in Fe5- x GeTe2 over a wide range of temperatures and probe their effects on thermal and electrical transport. A THE is detected, even at room T, that senses merons at higher T's, as well as their coexistence with skyrmions as T is lowered, indicating an on-demand thermally driven formation of either type of spin texture. Remarkably, an unconventional THE is also observed in absence of Lorentz force, and it is attributed to the interaction between charge carriers and magnetic field-induced chiral spin textures. These results expose Fe5-x GeTe2 as a promising candidate for the development of applications in skyrmionics/meronics due to the interplay between distinct but coexisting topological magnetic textures and unconventional transport of charge/heat carriers.

Thermal Hysteresis and Ordering Behavior of Magnetic Skyrmion Lattices.

The physics of phase transitions in two-dimensional (2D) systems underpins research in diverse fields including statistical mechanics, nanomagnetism, and soft condensed matter. However, many aspects of 2D phase transitions are still not well understood, including the effects of interparticle potential, polydispersity, and particle shape. Magnetic skyrmions are chiral spin-structure quasi-particles that form two-dimensional lattices. Here, we show, by real-space imaging using in situ cryo-Lorentz transmission electron microscopy coupled with machine learning image analysis, the ordering behavior of Néel skyrmion lattices in van der Waals Fe3GeTe2. We demonstrate a distinct change in the skyrmion size distribution during field-cooling, which leads to a loss of lattice order and an evolution of the skyrmion liquid phase. Remarkably, the lattice order is restored during field heating and demonstrates a thermal hysteresis. This behavior is explained by the skyrmion energy landscape and demonstrates the potential to control the lattice order in 2D phase transitions.

Freestanding Ferroelectric Bubble Domains.

Bubble-like domains, typically a precursor to the electrical skyrmions, arise in ultrathin complex oxide ferroelectric-dielectric-ferroelectric heterostructures epitaxially clamped with flat substrates. Here, it is reported that these specially ordered electric dipoles can also be retained in a freestanding state despite the presence of inhomogeneously distributed structural ripples. By probing local piezo and capacitive responses and using atomistic simulations, this study analyzes these ripples, sheds light on how the bubbles are stabilized in the modified electromechanical energy landscape, and discusses the difference in morphology between bubbles in freestanding and as-grown states. These results are anticipated to be the starting point of a new paradigm for the exploration of electric skyrmions with arbitrary boundaries and physically flexible topological orders in ferroelectric curvilinear space.

Mesoscale Confinement Effects and Emergent Quantum Interference in Titania Antidot Thin Films.

The effect of confinement on electron and ion transport in oxide films is of interest both fundamentally and technologically for the design of next-generation electronic devices. In metal oxides with mobile ions and vacancies, it is the interplay of the different modes of charge transport and the corresponding current-voltage signatures that is of interest. We developed a patterned structure in titania films, with feature sizes of 11-20 nm, that allow us to explore confined transport. We describe how confinement changes the competing charge transport mechanisms, the patterned antidot array leads to displacement fields and confines the charge density that results in modified and emergent electron transport with an increase in conductivity. This emergent behavior can be described by considering electron interference effects. Characterization of the charge transport with electron holography and impedance spectroscopy, and through comparison with modeling, show that nanoscale confinement is a way to control quantum interference.

The effect of annealing on optical transmittance and structure of ZLANI fluorozirconate glass thin films.

We report the effect of thermal annealing on structure, composition, optical transmittance and thickness of a novel fluorozirconate glass (ZLANI) containing Zr, La, Al, Na and In fluorides. In this work, pulsed laser deposition was used to grow thin films of ZLANI, and thermal annealing at different temperatures was performed on the films. Annealing did not change the composition, but a clear structural evolution of the ZLANI glass was observed by transmission electron microscopy (TEM), showing that we can control microstructure independent of composition. An increase in transmittance after the film was subject to a 100 °C thermal anneal was ascribed to the removal of defects and structural relaxation in the amorphous state. Following an anneal of 200 °C, the transmittance decreases due to heterogeneous formation of crystalline nuclei and changes in the local bonding. After the final annealing at 300 °C, a wider-scale crystallization occurred, with some major crystal phases formed as Zr2F8(H2O)6 and ZrO2, which alters the shape of the transmittance curve. The crystalline content of the crystal phases that form in the annealed films was quantified using hollow cone dark field TEM imaging. The 100 °C or 200 °C annealing decreases the film thickness by inducing structural relaxation and densification of the amorphous films, while the thickness increase of the 300 °C annealed film resulted from the formed large crystals. These results provide insights for the design of multilayer nanocomposites with a ZLANI glass matrix, which have potential applications as up-/down-conversion luminescent materials and X-ray storage phosphors.

Comparison of Metal Adhesion Layers for Au Films in Thermoplasmonic Applications.

If thermoplasmonic applications such as heat-assisted magnetic recording are to be commercially viable, it is necessary to optimize both thermal stability and plasmonic performance of the devices involved. In this work, a variety of different adhesion layers were investigated for their ability to reduce dewetting of sputtered 50 nm Au films on SiO2 substrates. Traditional adhesion layer metals Ti and Cr were compared with alternative materials of Al, Ta, and W. Film dewetting was shown to increase when the adhesion material diffuses through the Au layer. An adhesion layer thickness of 0.5 nm resulted in superior thermomechanical stability for all adhesion metals, with an enhancement factor of up to 200× over 5 nm thick analogues. The metals were ranked by their effectiveness in inhibiting dewetting, starting with the most effective, in the order Ta > Ti > W > Cr > Al. Finally, the Au surface-plasmon polariton response was compared for each adhesion layer, and it was found that 0.5 nm adhesion layers produced the best response, with W being the optimal adhesion layer material for plasmonic performance.

Ferroelectric Domain Wall Motion in Freestanding Single-Crystal Complex Oxide Thin Film.

Ferroelectric domain walls in single-crystal complex oxide thin films are found to be orders of magnitude slower when the interfacial bonds with the heteroepitaxial substrate are broken to create a freestanding film. This drastic change in domain wall kinetics does not originate from the alteration of epitaxial strain; rather, it is correlated with the structural ripples at mesoscopic length scale and associated flexoelectric effects induced in the freestanding films. In contrast, the effects of the bond-breaking on the local static ferroelectric properties of both top and bottom layers of the freestanding films, such as domain wall width and spontaneous polarization, are modest and governed by the change in epitaxy-induced compressive strain.

Less is More: Improved Thermal Stability and Plasmonic Response in Au Films via the Use of SubNanometer Ti Adhesion Layers.

The use of a metallic adhesion layer is known to increase the thermo-mechanical stability of Au thin films against solid-state dewetting, but in turn results in damping of the plasmonic response, reducing their utility in applications such as heat-assisted magnetic recording (HAMR). In this work, 50 nm Au films with Ti adhesion layers ranging in thickness from 0 to 5 nm were fabricated, and their thermal stability, electrical resistivity, and plasmonic response were measured. Subnanometer adhesion layers are demonstrated to significantly increase the stability of the thin films against dewetting at elevated temperatures (>200 °C), compared to more commonly used adhesion layer thicknesses that are in the range of 2-5 nm. For adhesion layers thicker than 1 nm, the diffusion of excess Ti through Au grain boundaries and subsequent oxidation was determined to result in degradation of the film. This mechanism was confirmed using transmission electron microscopy and X-ray photoelectron spectroscopy on annealed 0.5 and 5 nm adhesion layer samples. The superiority of subnanometer adhesion layers was further demonstrated through measurements of the surface-plasmon polariton resonance; those with thinner adhesion layers possessed both a stronger and spectrally sharper resonance. These results have relevance beyond HAMR to all Ti/Au systems operating at elevated temperatures.

Direct Evidence of Topological Defects in Electron Waves through Nanoscale Localized Magnetic Charge.

Topological concepts play an important role in, and provide unique insights into, many physical phenomena. In particular topological defects have become an active area of research due to their relevance to diverse systems including condensed matter and the early universe. These defects arise in systems during phase transitions or symmetry-breaking operations that lead to a specific configuration of the order parameter that is stable against external perturbations. In this work, we experimentally show that excitations or defects carrying magnetic charge in artificial spin ices introduce a topological defect in incident coherent electron waves. This results in the formation of a localized electron vortex beam carrying orbital angular momentum that is directly correlated with the magnetic charge. This work provides unique insight into the interaction of electrons with magnetically charged excitations and the effect on their topology thereby opening new possibilities to explore exotic scattering and quantum effects in nanoscale condensed-matter systems.

Ferroelectric Domain Studies of Patterned (001) BiFeO3 by Angle-Resolved Piezoresponse Force Microscopy.

We have studied the ferroelectric domains in (001) BiFeO3 (BFO) films patterned into mesas with various aspect ratios, using angle-resolved piezoresponse force microscope (AR-PFM), which can image the in-plane polarization component with an angular resolution of 30°. We observed not only stable polarization variants, but also meta-stable polarization variants, which can reduce the charge accumulated at domain boundaries. We considered the number of neighboring domains that are in contact, in order to analyze the complexity of the ferroelectric domain structure. Comparison of the ferroelectric domains from the patterned and unpatterned regions showed that the elastic relaxation induced by removal of the film surrounding the mesas led to a reduction of the average number of neighboring domains, indicative of a decrease in domain complexity. We also found that the rectangular BFO patterns with high aspect ratio had a simpler domain configuration and enhanced piezoelectric characteristics than square-shaped mesas. Manipulation of the ferroelectric domains by controlling the aspect ratio of the patterned BFO thin film mesas can be useful for nanoelectronic applications.

Interface-Induced Phenomena in Magnetism.

This article reviews static and dynamic interfacial effects in magnetism, focusing on interfacially-driven magnetic effects and phenomena associated with spin-orbit coupling and intrinsic symmetry breaking at interfaces. It provides a historical background and literature survey, but focuses on recent progress, identifying the most exciting new scientific results and pointing to promising future research directions. It starts with an introduction and overview of how basic magnetic properties are affected by interfaces, then turns to a discussion of charge and spin transport through and near interfaces and how these can be used to control the properties of the magnetic layer. Important concepts include spin accumulation, spin currents, spin transfer torque, and spin pumping. An overview is provided to the current state of knowledge and existing review literature on interfacial effects such as exchange bias, exchange spring magnets, spin Hall effect, oxide heterostructures, and topological insulators. The article highlights recent discoveries of interface-induced magnetism and non-collinear spin textures, non-linear dynamics including spin torque transfer and magnetization reversal induced by interfaces, and interfacial effects in ultrafast magnetization processes.