Low-Temperature ALD of SbOx /Sb2 Te3 Multilayers with Boosted Thermoelectric Performance.

Nanoscale superlattice (SL) structures have proven to be effective in enhancing the thermoelectric (TE) properties of thin films. Herein, the main phase of antimony telluride (Sb2 Te3 ) thin film with sub-nanometer layers of antimony oxide (SbOx ) is synthesized via atomic layer deposition (ALD) at a low temperature of 80 °C. The SL structure is tailored by varying the cycle numbers of Sb2 Te3 and SbOx . A remarkable power factor of 520.8 µW m-1 K-2 is attained at room temperature when the cycle ratio of SbOx and Sb2 Te3 is set at 1:1000 (i.e., SO:ST = 1:1000), corresponding to the highest electrical conductivity of 339.8 S cm-1 . The results indicate that at the largest thickness, corresponding to ten ALD cycles, the SbOx layers act as a potential barrier that filters out the low-energy charge carriers from contributing to the overall electrical conductivity. In addition to enhancing the scattering of the mid-to-long-wavelength at the SbOx /Sb2 Te3 interface, the presence of the SbOx sub-layer induces the confinement effect and strain forces in the Sb2 Te3 thin film, thereby effectively enhancing the Seebeck coefficient and reducing the thermal conductivity. These findings provide a new perspective on the design of SL-structured TE materials and devices.

Néel Skyrmion Bubbles in La0.7Sr0.3Mn1-xRuxO3 Multilayers.

Ferromagnetic La0.7Sr0.3Mn1-xRuxO3 epitaxial multilayers with controlled variation of the Ru/Mn content were synthesized to engineer canted magnetic anisotropy and variable exchange interactions, and to explore the possibility of generating a Dzyaloshinskii-Moriya interaction. The ultimate aim of the multilayer design is to provide the conditions for the formation of domains with nontrivial magnetic topology in an oxide thin film system. Employing magnetic force microscopy and Lorentz transmission electron microscopy in varying perpendicular magnetic fields, magnetic stripe domains separated by Néel-type domain walls as well as Néel skyrmions smaller than 100 nm in diameter were observed. These findings are consistent with micromagnetic modeling, taking into account a sizable Dzyaloshinskii-Moriya interaction arising from the inversion symmetry breaking and possibly from strain effects in the multilayer system.

Size-Specific Magnetic Configurations in Electrodeposited Epitaxial Iron Nanocuboids: From Landau Pattern to Vortex and Single Domain States.

As the size of magnetic devices continuously decreases, the creation of three-dimensional nanomagnets and the understanding of their magnetic configurations become increasingly important for modern applications. Here, by progressive nucleation during epitaxial nanoelectrodeposition, we synthesize single-crystal iron nanocuboids with sizes ranging 10 to 200 nm on one sample. The size-dependent magnetic configurations of these nanocuboids are studied by quantitative magnetic force microscopy and electron holography. In conjunction, a "magnetic configuration versus size" phase diagram is established via micromagnetic simulations. Both experiment and theory reveal a sequential transition from Landau pattern to vortex and finally single domain when decreasing the sizes of the nanocuboids. The combinatorial-like approach leads to a quantitative understanding of the magnetic configurations of the nanomagnets in a broad size range. It can be transferred to other materials and shapes and thereby presents an advanced route to enrich the material library for future nanodevice design.

Freestanding Nanolayers of a Wide-Gap Topological Insulator through Liquid-Phase Exfoliation.

The layered salt Bi14 Rh3 I9 is a weak three-dimensional (3D) topological insulator (TI), that is, a stack of two-dimensional (2D) TIs. It has a wide non-trivial band gap of 210 meV, which is generated by strong spin-orbit coupling, and possesses protected electronic edge-states. In the structure, charged layers of ∞ 2 [ (Bi4 Rh)3 I]2+ honeycombs and ∞ 1 [ Bi2 I8 ]2- chains alternate. The non-trivial topology of Bi14 Rh3 I9 is an inherent property of the 2D intermetallic fragment. Here, the exfoliation of Bi14 Rh3 I9 was performed using two different chemical approaches: (a) through a reaction with n-butyllithium and poly(vinylpyrrolidone), (b) through a reaction with betaine in dimethylformamide at 55 °C. The former yielded few-layer sheets of the new compound Bi12 Rh3 I, while the latter led to crystalline sheets of Bi14 Rh3 I9 with a thickness down to 5 nm and edge-lengths up to several ten microns. X-ray diffraction and electron microscopy proved that the structure of Bi14 Rh3 I9 remained intact. Thus, it was assumed that the particles are still TIs. Dispersions of these flakes now allow for next steps towards the envisioned applications in nanoelectronics, such as the study of quantum coherence in deposited films, the combination with superconducting particles or films for the generation of Majorana fermions, or studies on their behavior under the influence of magnetic or electric fields or in contact with various materials occurring in devices. The method presented generally allows to exfoliate layers with high specific charges and thus the use of layered starting materials beyond van der Waals crystals.

Three-Dimensional Imaging of Beam-Induced Biasing of InP/GaInP Tunnel Diodes.

Electron holographic tomography was used to obtain three-dimensional reconstructions of the morphology and electrostatic potential gradient of axial GaInP/InP nanowire tunnel diodes. Crystal growth was carried out in two opposite directions: GaInP-Zn/InP-S and InP-Sn/GaInP-Zn, using Zn as the p-type dopant in the GaInP but with changes to the n-type dopant (S or Sn) in the InP. Secondary electron and electron beam-induced current images obtained using scanning electron microscopy indicated the presence of p-n junctions in both cases and current-voltage characteristics measured via lithographic contacts showed the negative differential resistance, characteristic of band-to-band tunneling, for both diodes. Electron holographic tomography measurements confirmed a short depletion width in both cases (21 ± 3 nm) but different built-in potentials, Vbi, of 1.0 V for the p-type (Zn) to n-type (S) transition, and 0.4 V for both were lower than the expected 1.5 V for these junctions if degenerately doped. Charging induced by the electron beam was evident in phase images which showed nonlinearity in the surrounding vacuum, most severe in the case of the nanowire grounded at the p-type Au contact. We attribute their lower Vbi to asymmetric secondary electron emission, beam-induced current biasing, and poor grounding contacts.

Direct Observation of Plasmon Band Formation and Delocalization in Quasi-Infinite Nanoparticle Chains.

Chains of metallic nanoparticles sustain strongly confined surface plasmons with relatively low dielectric losses. To exploit these properties in applications, such as waveguides, the fabrication of long chains of low disorder and a thorough understanding of the plasmon-mode properties, such as dispersion relations, are indispensable. Here, we use a wrinkled template for directed self-assembly to assemble chains of gold nanoparticles. With this up-scalable method, chain lengths from two particles (140 nm) to 20 particles (1500 nm) and beyond can be fabricated. Electron energy-loss spectroscopy supported by boundary element simulations, finite-difference time-domain, and a simplified dipole coupling model reveal the evolution of a band of plasmonic waveguide modes from degenerated single-particle modes in detail. In striking difference from plasmonic rod-like structures, the plasmon band is confined in excitation energy, which allows light manipulations below the diffraction limit. The non-degenerated surface plasmon modes show suppressed radiative losses for efficient energy propagation over a distance of 1500 nm.

Three-Dimensional Composition and Electric Potential Mapping of III-V Core-Multishell Nanowires by Correlative STEM and Holographic Tomography.

The nondestructive characterization of nanoscale devices, such as those based on semiconductor nanowires, in terms of functional potentials is crucial for correlating device properties with their morphological/materials features, as well as for precisely tuning and optimizing their growth process. Electron holographic tomography (EHT) has been used in the past to reconstruct the total potential distribution in three-dimension but hitherto lacked a quantitative approach to separate potential variations due to chemical composition changes (mean inner potential, MIP) and space charges. In this Letter, we combine and correlate EHT and high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) tomography on an individual ⟨111⟩ oriented GaAs-AlGaAs core-multishell nanowire (NW). We obtain excellent agreement between both methods in terms of the determined Al concentration within the AlGaAs shell, as well as thickness variations of the few nanometer thin GaAs shell acting as quantum well tube. Subtracting the MIP determined from the STEM tomogram, enables us to observe functional potentials at the NW surfaces and at the Au-NW interface, both ascribed to surface/interface pinning of the semiconductor Fermi level.

Synthesis and Three-Dimensional Magnetic Field Mapping of Co2FeGa Heusler Nanowires at 5 nm Resolution.

We present the synthesis of Co2FeGa Heusler nanowires and the results of our investigations on their three-dimensional (3D) electric and magnetic internal and external fields mapped by electron holographic tomography (EHT). These fields will be of great importance in next-generation nanomagnets integrated in spintronics and memory devices. The Co2FeGa nanowires with a L21 ordered structure are prepared by a SBA-15 silica-assisted method. The magnetic dipole-like stray fields of several Co2FeGa nanowires are revealed by holographically reconstructed phase images. Based on the measured magnetic phase shifts of an individual nanowire and its 3D reconstruction using EHT, we obtain an internal magnetic induction with a magnitude of 1.15 T and a nonmagnetic surface layer of 10 nm thickness. Furthermore, we also reconstruct the 3D distribution of the electrostatic potential of the same nanowire.

Elastic Scattering of Electron Vortex Beams in Magnetic Matter.

Elastic scattering of electron vortex beams on magnetic materials leads to a weak magnetic contrast due to Zeeman interaction of orbital angular momentum of the beam with magnetic fields in the sample. The magnetic signal manifests itself as a redistribution of intensity in diffraction patterns due to a change of sign of the orbital angular momentum of the electron vortex beam. While in the atomic resolution regime the magnetic signal is most likely under the detection limits of present transmission electron microscopes, for electron probes with high orbital angular momenta, and correspondingly larger spatial extent, its detection is predicted to be feasible.

Interfacial Distortion of Sb2Te3-Sb2Se3 Multilayers via Atomic Layer Deposition for Enhanced Thermoelectric Properties.

Atomic layer deposition (ALD) is an effective technique for depositing thin films with precise control of layer thickness and functional properties. In this work, Sb2Te3-Sb2Se3 nanostructures were synthesized using thermal ALD. A decrease in the Sb2Te3 layer thickness led to the emergence of distinct peaks from the Laue rings, indicative of a highly textured film structure with optimized crystallinity. Density functional theory simulations revealed that carrier redistribution occurs at the interface to establish charge equilibrium. By carefully optimizing the layer thicknesses, we achieved an obvious enhancement in the Seebeck coefficient, reaching a peak figure of merit (zT) value of 0.38 at room temperature. These investigations not only provide strong evidence for the potential of ALD manipulation to improve the electrical performance of metal chalcogenides but also offer valuable insights into achieving high performance in two-dimensional materials.

Transport of intensity phase retrieval of arbitrary wave fields including vortices.

The phase problem can be considered as one of the cornerstones of quantum mechanics intimately connected to the detection process and the uncertainty relation. The latter impose fundamental limits on the manifold phase reconstruction schemes invented to date, in particular, at small magnitudes of the quantum wave. Here, we show that a rigorous solution of the transport of intensity reconstruction (TIE) scheme in terms of a linear elliptic partial differential equation for the phase provides reconstructions even in the presence of wave zeros if particular boundary conditions are given. We furthermore discuss how partial coherence hampers phase reconstruction and show that a modified version of the TIE reconstructs the curl-free current density at arbitrary (in)coherence. Our results open the way for TIE-based phase retrieval of arbitrary wave fields, eventually containing zeros such as phase vortices.

WRAP: A wavelet-regularised reconstruction algorithm for magnetic vector electron tomography.

Magnetic vector electron tomography (VET) is a promising technique that enables better understanding of micro- and nano-magnetic phenomena through the reconstruction of 3D magnetic fields at high spatial resolution. Here we introduce WRAP (Wavelet Regularised A Program), a reconstruction algorithm for magnetic VET that directly reconstructs the magnetic vector potential A using a compressed sensing framework which regularises for sparsity in the wavelet domain. We demonstrate that using WRAP leads to a significant increase in the fidelity of the 3D reconstruction and is especially robust when dealing with very limited data; using datasets simulated with realistic noise, we compare WRAP to a conventional reconstruction algorithm and find an improvement of ca. 60% when averaged over several performance metrics. Moreover, we further validate WRAP's performance on experimental electron holography data, revealing the detailed magnetism of vortex states in a CuCo nanowire. We believe WRAP represents a major step forward in the development of magnetic VET as a tool for probing magnetism at the nanoscale.

Chirality coupling in topological magnetic textures with multiple magnetochiral parameters.

Chiral effects originate from the lack of inversion symmetry within the lattice unit cell or sample's shape. Being mapped onto magnetic ordering, chirality enables topologically non-trivial textures with a given handedness. Here, we demonstrate the existence of a static 3D texture characterized by two magnetochiral parameters being magnetic helicity of the vortex and geometrical chirality of the core string itself in geometrically curved asymmetric permalloy cap with a size of 80 nm and a vortex ground state. We experimentally validate the nonlocal chiral symmetry breaking effect in this object, which leads to the geometric deformation of the vortex string into a helix with curvature 3 µm-1 and torsion 11 µm-1. The geometric chirality of the vortex string is determined by the magnetic helicity of the vortex texture, constituting coupling of two chiral parameters within the same texture. Beyond the vortex state, we anticipate that complex curvilinear objects hosting 3D magnetic textures like curved skyrmion tubes and hopfions can be characterized by multiple coupled magnetochiral parameters, that influence their statics and field- or current-driven dynamics for spin-orbitronics and magnonics.

Multiscale Reciprocal Space Mapping of Magnetite Mesocrystals.

Mesocrystals are a class of nanostructured material, where a multiple-length-scale structure is a prerequisite of many interesting phenomena. Resolving the mesocrystal structure is quite challenging due to their structuration on different length scales. The combination of small- and wide-angle X-ray scattering (SAXS and WAXS) techniques offers the possibility of non-destructively probing mesocrystalline structures simultaneously, over multiple length scales to reveal their microscopic structure. This work describes how high dynamical range of modern detectors sheds light on the weak features of scattering, significantly increasing the information content. The detailed analysis of X-ray diffraction (XRD) from the magnetite mesocrystals with different particle sizes and shapes is described, in tandem with electron microscopy. The revealed features provide valuable input to the models of mesocrystal growth and the choice of structural motif; the impact on magnetic properties is discussed.

Hierarchically Engineered Manganite Thin Films with a Wide-Temperature-Range Colossal Magnetoresistance Response.

Colossal magnetoresistance is of great fundamental and technological significance in condensed-matter physics, magnetic memory, and sensing technologies. However, its relatively narrow working temperature window is still a severe obstacle for potential applications due to the nature of the material-inherent phase transition. Here, we realized hierarchical La0.7Sr0.3MnO3 thin films with well-defined (001) and (221) crystallographic orientations by combining substrate modification with conventional thin-film deposition. Microscopic investigations into its magnetic transition through electron holography reveal that the hierarchical microstructure significantly broadens the temperature range of the ferromagnetic-paramagnetic transition, which further widens the response temperature range of the macroscopic colossal magnetoresistance under the scheme of the double-exchange mechanism. Therefore, this work puts forward a method to alter the magnetic transition and thus to extend the magnetoresistance working window by nanoengineering, which might be a promising approach also for other phase-transition-related effects in functional oxides.

Unveiling the three-dimensional magnetic texture of skyrmion tubes.

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.

Observation of fractional spin textures in a Heusler material.

Recently a zoology of non-collinear chiral spin textures has been discovered, most of which, such as skyrmions and antiskyrmions, have integer topological charges. Here we report the experimental real-space observation of the formation and stability of fractional antiskyrmions and fractional elliptical skyrmions in a Heusler material. These fractional objects appear, over a wide range of temperature and magnetic field, at the edges of a sample, whose interior is occupied by an array of nano-objects with integer topological charges, in agreement with our simulations. We explore the evolution of these objects in the presence of magnetic fields and show their interconversion to objects with integer topological charges. This means the topological charge can be varied continuously. These fractional spin textures are not just another type of skyrmion, but are essentially a new state of matter that emerges and lives only at the boundary of a magnetic system. The coexistence of both integer and fractionally charged spin textures in the same material makes the Heusler family of compounds unique for the manipulation of the real-space topology of spin textures and thus an exciting platform for spintronic and magnonic applications.

Flexomagnetism and vertically graded Néel temperature of antiferromagnetic Cr2O3 thin films.

Antiferromagnetic insulators are a prospective materials platform for magnonics, spin superfluidity, THz spintronics, and non-volatile data storage. A magnetomechanical coupling in antiferromagnets offers vast advantages in the control and manipulation of the primary order parameter yet remains largely unexplored. Here, we discover a new member in the family of flexoeffects in thin films of Cr2O3. We demonstrate that a gradient of mechanical strain can impact the magnetic phase transition resulting in the distribution of the Néel temperature along the thickness of a 50-nm-thick film. The inhomogeneous reduction of the antiferromagnetic order parameter induces a flexomagnetic coefficient of about 15 µB nm-2. The antiferromagnetic ordering in the inhomogeneously strained films can persist up to 100 °C, rendering Cr2O3 relevant for industrial electronics applications. Strain gradient in Cr2O3 thin films enables fundamental research on magnetomechanics and thermodynamics of antiferromagnetic solitons, spin waves and artificial spin ice systems in magnetic materials with continuously graded parameters.

Extraction of physically meaningful endmembers from STEM spectrum-images combining geometrical and statistical approaches.

This article addresses extraction of physically meaningful information from STEM EELS and EDX spectrum-images using methods of Multivariate Statistical Analysis. The problem is interpreted in terms of data distribution in a multi-dimensional factor space, which allows for a straightforward and intuitively clear comparison of various approaches. A new computationally efficient and robust method for finding physically meaningful endmembers in spectrum-image datasets is presented. The method combines the geometrical approach of Vertex Component Analysis with the statistical approach of Bayesian inference. The algorithm is described in detail at an example of EELS spectrum-imaging of a multi-compound CMOS transistor.

Correction: Exploring the 3D structure and defects of a self-assembled gold mesocrystal by coherent X-ray diffraction imaging.

Correction for 'Exploring the 3D structure and defects of a self-assembled gold mesocrystal by coherent X-ray diffraction imaging' by Jerome Carnis et al., Nanoscale, 2021, DOI: 10.1039/D1NR01806J.