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Mg-doped, graded AlGaN films showed the formation of an impurity band and high, temperature-invariant p-conductivity even for doping levels well below the Mott transition. However, compensating point defects disrupted the impurity band, resulting in an Anderson transition from the impurity band to valence band conduction and a more than tenfold reduction in room-temperature conductivity. This is the first demonstration of Anderson-like localization in AlGaN films. [ABSTRACT FROM AUTHOR]

We demonstrate a pathway employing crystal polarity controlled asymmetric impurity incorporation in the wide bandgap nitride material system to enable 3D doping control during the crystal growth process. The pathway involves polarity specific supersaturation modulated growth of lateral polar structures of alternating Ga- and N-polar GaN domains. A STEM technique of integrated differential phase contrast is used to image the atomic structure of the different polar domains and their single atomic plane boundaries. As a demonstration, 1 μm wide alternating Ga- and N-polar GaN domains exhibiting charge balanced and periodic domains for superjunction technology were grown. The challenges in characterizing the resulting 3D doping profile were addressed with atom probe tomography with atomic scale compositional resolution corroborating capacitance measurements and secondary-ion mass spectroscopy analysis. [ABSTRACT FROM AUTHOR]

Magnetic transition metal chalcogenides form an emerging platform for exploring spin-orbit driven Berry phase phenomena owing to the nontrivial interplay between topology and magnetism. Here we show that the anomalous Hall effect in pristine Cr2Te3 thin films manifests a unique temperature-dependent sign reversal at nonzero magnetization, resulting from the momentum-space Berry curvature as established by first-principles simulations. The sign change is strain tunable, enabled by the sharp and well-defined substrate/film interface in the quasi-two-dimensional Cr2Te3 epitaxial films, revealed by scanning transmission electron microscopy and depth-sensitive polarized neutron reflectometry. This Berry phase effect further introduces hump-shaped Hall peaks in pristine Cr2Te3 near the coercive field during the magnetization switching process, owing to the presence of strain-modulated magnetic layers/domains. The versatile interface tunability of Berry curvature in Cr2Te3 thin films offers new opportunities for topological electronics. Chromium tellurides are a particularly promising family of quasi-2D magnetic materials; towards the single van der Waals layer limit, they preserve magnetic ordering, some even above room temperature, and exhibit a variety of intrinsic topological properties. Here, Hang Chi, Yunbo Ou and co-authors demonstrate a strain tunable Berry curvature induced reversal of the anomalous Hall effect in Cr2Te3. [ABSTRACT FROM AUTHOR]

Diffraction analysis in four-dimensional scanning transmission electron microscopy now enables the mapping of local structures including symmetry, strain, and polarization of materials. However, measuring the distribution of these configurations at the unit cell level remains a challenge because most analysis methods require the diffraction disks to be separated, limiting the electron probe sizes to be larger than a unit cell. Here, we show improved spatial resolution in mapping the polarization displacement and phases of BaTiO3 sampled at a rate equivalent to the size of the projected unit cells using 4D-STEM. This improvement in spatial resolution is accomplished by masking out the overlapping regions in partially overlapped convergent beam electron diffraction patterns. By reducing the probe size to the order of single projected unit cells in size, the measurement shows local fluctuation within the nanosized rhombohedral domains in tetragonal phased BaTiO3, indicating the origin of phase transition and evolution across different length scales. [ABSTRACT FROM AUTHOR]

H2W2O7, a metastable material synthesized via selective etching of the Aurivillius‐related Bi2W2O9, is demonstrated as an electrode for high power proton‐based energy storage. Comprehensive structural characterization is performed to obtain a high‐fidelity crystal structure of H2W2O7 using an iterative approach that combines X‐ray diffraction, neutron pair distribution function, scanning transmission electron microscopy, Raman spectroscopy, and density functional theory modeling. Electrochemical characterization shows a capacity retention of ≈80% at 1000 mV s–1 (1.5‐s charge/discharge time) as compared to 1 mV s–1 (≈16‐min charge/discharge time) with cyclability for over 100 000 cycles. Energetics from density functional theory calculations indicate that proton storage occurs at the terminal oxygen sites within the hydrated interlayer. Last, optical micrographs collected during in situ Raman spectroscopy show reversible, multicolor electrochromism, with color changes from pale yellow to blue, purple, and last, orange as a function of proton content. These results highlight the use of selective etching of layered perovskites for the synthesis of metastable transition metal oxide materials and the use of H2W2O7 as an anode material for proton‐based energy storage or electrochromic applications. [ABSTRACT FROM AUTHOR]

Device quality InGaN templates are synthesized using the semibulk (SB) approach. The approach maintains the film's 2D growth and avoids the formation of indium-metal inclusions. The strain relaxation processes of the grown InxGa1−xN templates are accompanied by variations in the indium content (x) and lattice parameters (a and c) across the InGaN template's thickness as the residual strain is continuously decreasing. This strain and lattice parameters' variation creates difficulties in applying standard x-ray Diffraction (XRD) and Reciprocal Space mapping (RSM) techniques to estimate the residual strain and the degree of the elastic strain relaxation. We used high-resolution High-angle annular dark-field scanning transmission electron microscopy and Energy-dispersive x-ray spectroscopy (EDS) to monitor the variations of the indium content, lattice parameters, and strain relaxation across the growing InxGa1−xN templates. We show that strain relaxation takes place by V-pit defect formation. Some of these V-pits are refilled by the GaN interlayers in the InxGa1−xN SB templates, while others propagate to the template surface. We present an alternative approach combining photoluminescence (PL) and EDS for estimating the degree of strain relaxation in these InxGa1−xN templates. The values obtained for the degree of relaxation estimated from TEM studies and PL measurements are within reasonable agreement in this study. Device quality InxGa1−xN templates with x ∼ 0.08, with a degree of relaxation higher than 70%, are achieved. [ABSTRACT FROM AUTHOR]

The mechanisms governing "compositional pulling" during the growth of AlxGa1−xN wells are investigated. Gallium-rich AlxGa1−xN wells grown on high dislocation density AlN/sapphire templates exhibit asymmetric and diffuse composition profiles, while those grown on low dislocation density native AlN substrates do not. Furthermore, strain in all AlxGa1−xN wells is found to be pseudomorphic, ruling it out as the dominating driving force. Rather, the high threading dislocation density of the AlN template is considered to play the defining role. We propose that a transient surface morphology is introduced during dislocation mediated spiral growth, which, in conjunction with process supersaturation, determines the Ga incorporation. These findings provide insights into compositional pulling in high Ga content AlxGa1−xN grown on AlN and provide a route to grow thicker wells with very abrupt interfaces on native AlN substrates. [ABSTRACT FROM AUTHOR]

The article discusses Oxidative dehydrogenation of n-butane has the potential to efficiently produce butadiene without equilibrium limitation or coke formation. Despite extensive research efforts, single-pass butadiene yields are limited to <23% in conventional catalytic ODH with gaseous O2. This article reports molten LiBr as an effective promoter to modify a redox-active perovskite oxide, i.e., La0.8Sr0.2FeO3.

The direct observation of a solid-state chemical reaction can reveal otherwise hidden mechanisms that control the reaction kinetics. However, probing the chemical bond breaking and formation at the molecular level remains challenging because of the insufficient spatial-temporal resolution and composition analysis of available characterization methods. Using atomic-resolution differential phase-contrast imaging in scanning transmission electron microscopy, we have visualized the decomposition chemistry of K 2 PtCl 4 to identify its transient intermediate phases and their interfaces that characterize the chemical reduction process. The crystalline structure of K 2 PtCl 4 is found to undergo a disproportionation reaction to form K 2 PtCl 6 , followed by gradual reduction to crystalline Pt metal and KCl. By directly imaging different Pt─Cl bond configurations and comparing them to models predicted via density functional theory calculations, a causal connection between the initial and final states of a chemical reaction is established, showcasing new opportunities to resolve reaction pathways through atomistic experimental visualization.

Transmission electron microscopy (TEM) enables users to study materials at their fundamental, atomic scale. Complex experiments routinely generate thousands of images with numerous parameters that require time-consuming and complicated analysis. AXON synchronicity is a machine-vision synchronization (MVS) software solution designed to address the pain points inherent to TEM studies. Once installed on the microscope, it enables the continuous synchronization of images and metadata generated by the microscope, detector, and in situ systems during an experiment. This connectivity enables the application of machine-vision algorithms that apply a combination of spatial, beam, and digital corrections to center and track a region of interest within the field of view and provide immediate image stabilization. In addition to the substantial improvement in resolution afforded by such stabilization, metadata synchronization enables the application of computational and image analysis algorithms that calculate variables between images. This calculated metadata can be used to analyze trends or identify key areas of interest within a dataset, leading to new insights and the development of more sophisticated machine-vision capabilities in the future. One such module that builds on this calculated metadata is dose calibration and management. The dose module provides state-of-the-art calibration, tracking, and management of both the electron fluence (e - /Å 2 ·s -1 ) and cumulative dose (e - /Å 2 ) that is delivered to specific areas of the sample on a pixel-by-pixel basis. This enables a comprehensive overview of the interaction between the electron beam and the sample. Experiment analysis is streamlined through a dedicated analysis software in which datasets consisting of images and corresponding metadata are easily visualized, sorted, filtered, and exported. Combined, these tools facilitate efficient collaborations and experimental analysis, encourage data mining and enhance the microscopy experience.

Oxidative dehydrogenation (ODH) of n -butane has the potential to efficiently produce butadiene without equilibrium limitation or coke formation. Despite extensive research efforts, single-pass butadiene yields are limited to <23% in conventional catalytic ODH with gaseous O 2 . This article reports molten LiBr as an effective promoter to modify a redox-active perovskite oxide, i.e., La 0.8 Sr 0.2 FeO 3 (LSF), for chemical looping-oxidative dehydrogenation of n -butane (CL-ODHB). Under the working state, the redox catalyst is composed of a molten LiBr layer covering the solid LSF substrate. Characterizations and ab initio molecular dynamics (AIMD) simulations indicate that peroxide species formed on LSF react with molten LiBr to form active atomic Br, which act as reaction intermediates for C─H bond activation. Meanwhile, molten LiBr layer inhibits unselective CO 2 formation, leading to 42.5% butadiene yield. The redox catalyst design strategy can be extended to CL-ODH of other light alkanes such as iso -butane conversion to iso -butylene, providing a generalized approach for olefin production.

As human health concerns over disinfection byproducts (DBP) in drinking water increase, so does the need to develop new materials that remove them rapidly and at high capacity. Ion exchange (IEX) is an effective method for the removal of natural organic matter (NOM), especially anion exchange resins (AERs) with quaternary ammonium functional groups. However, capacity is limited in existing commercial resin materials because adsorbates can only interact with the outermost surface area, which makes these products inefficient on a mass basis. We have synthesized a novel "NanoResin" exploiting the enhanced NOM removal of the quaternary ammonium resin while utilizing the vast surface area of SWCNTs, which act as scaffolding for the resin. Our nanomaterials show increased adsorption capacity compared to commercially available adsorbents, in a fraction of the time. This NanoResin requires only about 10 s to reach ion-exchange equilibrium. Comparatively, commercial AERs only achieved partial removal after more than 30 min. High capacity adsorption of a low molecular weight (MW) surrogate has been measured. NOM removal was demonstrated in solutions of both low and high specific UV absorbance (SUVA) composition with these nanomaterials. Additionally, the NanoResin showed enhanced removal of a NOM concentrate sample taken from Myrtle Beach, SC, demonstrating NanoResin is an effective method of removal for refractory NOM in a natural aqueous environment. Synthesis and characterization of the polymers and nanomaterials are presented below. Adsorption capacity, adsorption kinetics, and the regeneration and reusability of these new materials for NOM removal are described. The open matrix microstructure precludes any intraparticle diffusion of adsorbates; thus, these nanomaterials act as a "contact resin".