Counting Point Defects at Nanoparticle Surfaces by Electron Holography.

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

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

We report a magnetic transition region in La_{0.7}Sr_{0.3}MnO_{3} with gradually changing magnitude of magnetization, but no rotation, stable at all temperatures below T_{C}.

Electron-beam-induced charging of an AlO nanotip studied using off-axis electron holography.

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 AlO nanotip on a conducting support.

Synergistic use of gradient flipping and phase prediction for inline electron holography.

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.

Nanoscale visualization of metallic electrodeposition in a well-controlled chemical environment.

Liquid phase transmission electron microscopy (TEM) provides a useful means to study a wide range of dynamics in solution with near-atomic spatial resolution and sub-microsecond temporal resolution. However, it is still a challenge to control the chemical environment (such as the flow of liquid, flow rate, and the liquid composition) in a liquid cell, and evaluate its effect on the various dynamic phenomena. In this work, we have systematically demonstrated the flow performance of anliquid TEM system, which is based on 'on-chip flow' driven by external pressure pumps.

Low-Pt NiNC-Supported PtNi Nanoalloy Oxygen Reduction Reaction Electrocatalysts-In Situ Tracking of the Atomic Alloying Process.

We report and analyze a synthetic strategy toward low-Pt platinum-nickel (Pt-Ni) alloy nanoparticle (NP) cathode catalysts for the catalytic electroreduction of molecular oxygen to water. The synthesis involves the pyrolysis and leaching of Ni-organic polymers, subsequent Pt NP deposition, followed by thermal alloying, resulting in single Ni atom site (NiNC)-supported PtNi alloy NPs at low Pt weight loadings of only 3-5 wt %. Despite low Pt weight loading, the catalysts exhibit more favorable Pt-mass activities compared to conventional 20-30 wt % benchmark PtNi catalysts.

Highly Active and Stable Large Mo-Doped Pt-Ni Octahedral Catalysts for ORR: Synthesis, Post-treatments, and Electrochemical Performance and Stability.

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.

Ductile deformation during carbonation of serpentinized peridotite.

Carbonated serpentinites (listvenites) in the Samail Ophiolite, Oman, record mineralization of 1-2 Gt of CO, but the mechanisms providing permeability for continued reactive fluid flow are unclear. Based on samples of the Oman Drilling Project, here we show that listvenites with a penetrative foliation have abundant microstructures indicating that the carbonation reaction occurred during deformation. Folded magnesite veins mark the onset of carbonation, followed by deformation during carbonate growth.

Active Interphase Enables Stable Performance for an All-Phosphate-Based Composite Cathode in an All-Solid-State Battery.

High interfacial resistance and unstable interphase between cathode active materials (CAMs) and solid-state electrolytes (SSEs) in the composite cathode are two of the main challenges in current all-solid-state batteries (ASSBs). In this work, the all-phosphate-based LiFePO (LFP) and Li Al Ti (PO ) (LATP) composite cathode is obtained by a co-firing technique. Benefiting from the densified structure and the formed redox-active Li Fe Ti Al (PO ) (LFTAP) interphase, the mixed ion- and electron-conductive LFP/LATP composite cathode facilitates the stable operation of bulk-type ASSBs in different voltage ranges with almost no capacity degradation upon cycling.

Highly complex magnetic behavior resulting from hierarchical phase separation in AlCo(Cr)FeNi high-entropy alloys.

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 AlCoCrFeNi 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.

Impact of Molecule Concentration, Diffusion Rates and Surface Passivation on Single-Molecule Fluorescence Studies in Solution.

For single-molecule studies in solution, very small concentrations of dye-labelled molecules are employed in order to achieve single-molecule sensitivity. In typical studies with confocal microscopes, often concentrations in the pico-molar regime are required. For various applications that make use of single-molecule Förster resonance energy transfer (smFRET) or two-color coincidence detection (TCCD), the molecule concentration must be set explicitly to targeted values and furthermore needs to be stable over a period of several hours.

A transmission electron microscopy study of low-strain epitaxial BaTiOgrown onto NdScO.

Ferroelectric materials exhibit a strong coupling between strain and electrical polarization. In epitaxial thin films, the strain induced by the substrate can be used to tune the domain structure. Substrates of rare-earth scandates are sometimes selected for the growth of ferroelectric oxides because of their close lattice match, which allows the growth of low-strain dislocation-free layers.

Water-Based Synthesis of Ultrasmall Nanoparticles of Platinum Group Metal Oxides (1.8 nm).

Ultrasmall nanoparticles of platinum group metal oxides (core diameter of about 1.8 nm) were prepared by alkaline hydrolysis of metal precursors in the presence of NaBH and by colloidal stabilization with tripeptide glutathione. We obtained water-dispersed nanoparticles of RhO, PdO, RuO, IrO, Os/OsO, and Pt/PtO.

transmission electron microscopy of battery cycling: thickness dependent breaking of TiO coating on Si/SiO nanoparticles.

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 transmission electron microscopy in an open cell to show that TiO coatings on Si/SiO 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.

Prospect for measuring two-dimensional van der Waals magnets by electron magnetic chiral dichroism.

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.

Atomic-Scale Insights into Nickel Exsolution on LaNiO Catalysts via Electron Microscopy.

Using a combination of bulk and surface characterization techniques, we provide atomic-scale insight into the complex surface and bulk dynamics of a LaNiO perovskite material during heating . Driven by the outstanding activity LaNiO in the methane dry reforming reaction (DRM), attributable to the decomposition of LaNiO during DRM operation into a Ni//LaO composite, we reveal the Ni exsolution dynamics both on a local and global scale by electron microscopy, X-ray diffraction and 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.

A High Conductivity 1D π-d Conjugated Metal-Organic Framework with Efficient Polysulfide Trapping-Diffusion-Catalysis in Lithium-Sulfur Batteries.

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.

Continuous illumination picosecond imaging using a delay line detector in a transmission electron microscope.

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.

Measurement of polarization effects in dual-phase ceria-based oxygen permeation membranes using Kelvin probe force microscopy.

In this study, a dual phase composite (CSO-FC2O) consisting of 60 vol % CeSmO as oxygen-conductive phase and 40 vol % FeCoO as electron-conductive phase was synthesized. TEM measurements showed a relatively pure dual-phase material with only minor amounts of a tertiary (Sm,Ce)(Fe,Co)O perovskite phase and isolated residues of a rock salt phase at the grain boundaries. The obtained material was used as a model to demonstrate that a combination of polarization relaxation measurements and Kelvin probe force microscopy (KPFM)-based mapping of the Volta potential before and after the end of polarization can be used to determine the chemical diffusion coefficient of the ceria component of the composite.

Structural Phase Transition and In-Situ Energy Storage Pathway in Nonpolar Materials: A Review.

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.

Shaping of Electron Beams Using Sculpted Thin Films.

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.

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.

Dynamical diffraction of high-energy electrons investigated by focal series momentum-resolved scanning transmission electron microscopy at atomic resolution.

We report a study of scattering dynamics in crystals employing momentum-resolved scanning transmission electron microscopy under varying illumination conditions. As we perform successive changes of the probe focus, multiple real-space signals are obtained in dependence of the shape of the incident electron wave. With support from extensive simulations, each signal is shown to be characterised by an optimum focus for which the contrast is maximum and which differs among different signals.