The catalytic activity of heterogeneous catalysts is significantly influenced by strong metal-support interaction (SMSI), which markedly alters their structure and electronic states. Direct observation of atomic-scale structural changes associated with SMSI can provide critical insights into the catalytic performance enhancements. However, few studies have captured the atomic-scale dynamics under close to realistic conditions. In this study, we integrated atomic-resolution scanning transmission electron microscopy with in situ observations of 1-2 nm Pt nanoparticles on anatase TiO2(101) under quasi-atmospheric and high-temperature conditions, enabling direct visualization of the structural transformations associated with SMSI. Under these conditions, the formation of oxygen vacancies triggered Pt-Ti alloy formation accompanied by a change in the Pt/TiO2 interfacial orientation relationship within the nanoparticles. Our findings provide valuable insights into the atomic-scale mechanisms governing catalytic activity, potentially contributing to the rational design of high-performance catalysts.

Understanding the intrinsic degradation processes of organic light-emitting diodes is necessary to improve their lifetimes. This intrinsic degradation is typically caused by carrier injection at the interface between the hole transport layer (HTL) and the emissive layer (EML). However, revealing the charge behavior in this local region with a high spatial resolution remains challenging. Thus, this study employed electron holography, a transmission electron microscopy (TEM) technique, to measure the nanometer scale potential distribution inside an OLED composed of N,N '-di-[(1-naphthyl)-N,N '-diphenyl]-(1,1 '-biphenyl)-4,4 '-diamine (alpha-NPD) and tris-(8-hydroxyquinoline)aluminum (Alq3) that was degraded via continuous voltage application. The alpha-NPD and Alq3 functioned as the HTL and EML, respectively. The degraded OLED was found to exhibit several potential distributions, depending on the local positions from which the TEM samples were lifted out of the same bulk sample. The distributions included (i) formation of a potential valley at the alpha-NPD/Alq3 interface, (ii) disappearance of electric fields within the organic layers, and (iii) similar distribution to original before degradation. We suggest that the degradation was caused by charge accumulation, cationization of Alq3, and local failures. Thus, this study revealed the influence of electric degradation at the nanometer scale because of charge injection to the alpha-NPD/Alq3 interface. Electron holographic degradation analysis near the HTL/EML interface is expected to aid in the development of design guidelines for preventing device degradation and thus extend device lifetime.

Abstract Extraterrestrial minerals on the surface of airless Solar System bodies undergo gradual alteration processes known as space weathering over long periods of time. The signatures of space weathering help us understand the phenomena occurring in the Solar System. However, meteorites rarely retain the signatures, making it impossible to study the space weathering processes precisely. Here, we examine samples retrieved from the asteroid Ryugu by the Hayabusa2 spacecraft and discover the presence of nonmagnetic framboids through electron holography measurements that can visualize magnetic flux. Magnetite particles, which normally provide a record of the nebular magnetic field, have lost their magnetic properties by reduction via a high-velocity (>5 km s–1) impact of a micrometeoroid with a diameter ranging from 2 to 20 μm after destruction of the parent body of Ryugu. Around these particles, thousands of metallic-iron nanoparticles with a vortex magnetic domain structure, which could have recorded a magnetic field in the impact event, are found. Through measuring the remanent magnetization of the iron nanoparticles, future studies are expected to elucidate the nature of the nebular/interplanetary magnetic fields after the termination of aqueous alteration in an asteroid.

Atomic-resolution scanning transmission electron microscopy combined with 2D Gaussian fitting enables the accurate and precise identification of atomic column positions within a few picometers. The measurement performance significantly depends on the signal-to-noise ratio of the atomic columns. In areas with low signal-to-noise ratios, such as near surfaces, the measurement performance was lower than that of the bulk. However, previous studies evaluated the accuracy and precision only in bulk areas, underscoring the need for a method that quantitatively evaluates the accuracy and precision of each atomic column position with various signal-to-noise ratios. This study introduced Bayesian inference to assess the accuracy and precision of determining individual atomic column positions under various signals. We applied this method to simulated and experimental images and demonstrated its effectiveness in identifying statistically significant displacements, particularly near surfaces with signal degradation. The use of vector maps and kernel density estimate plots obtained from Bayesian inference provided a probabilistic understanding of the atom displacement. Therefore, this study highlighted the potential benefits of Bayesian inference in high-resolution imaging to reveal material properties.

Plasmonic Schottky devices have attracted considerable attention for use in practical applications based on photoelectric conversion, because they enable light to be harvested below the bandgap of semiconductors. In particular, silicon-based (Si) plasmonic Schottky devices have great potential for useful photodetection in the near-infrared region. However, the internal quantum efficiency (IQE) values of previously reported devices are low because the Schottky barrier is excessively high. Here, we are the first to develop AuAg nanoalloy-n-type Si plasmonic Schottky devices by cathodic arc plasma deposition. Interestingly, it is found that a novel nanostructure, which leads to the improvement of responsivities, is formed. Moreover, these plasmonic nanostructures can be fabricated in only similar to 1 min. The fabricated AuAg nanoparticle-film structure enables proper control of the Schottky barrier height and increases the area of the Schottky interface for electron transfer. As a result, the considerably enhanced IQE of our device at a telecommunication wavelength of 1310 nm (1550 nm) without external bias is 4.6 (6.5) times higher than those in previous reports, and these responsivities are a record high. This approach can be applied to realize efficient photodetection in the NIR region and extend the use of light below the bandgap of semiconductors. This paves the way for future application advancements in a variety of fields, including photodetection, imaging, photovoltaics, and photochemistry.

Samples of the carbonaceous asteroid Ryugu were brought to Earth by the Hayabusa2 spacecraft. We analyzed 17 Ryugu samples measuring 1 to 8 millimeters. Carbon dioxide-bearing water inclusions are present within a pyrrhotite crystal, indicating that Ryugu's parent asteroid formed in the outer Solar System. The samples contain low abundances of materials that formed at high temperatures, such as chondrules and calcium- and aluminum-rich inclusions. The samples are rich in phyllosilicates and carbonates, which formed through aqueous alteration reactions at low temperature, high pH, and water/rock ratios of <1 (by mass). Less altered fragments contain olivine, pyroxene, amorphous silicates, calcite, and phosphide. Numerical simulations, based on the mineralogical and physical properties of the samples, indicate that Ryugu's parent body formed ~2 million years after the beginning of Solar System formation.

To improve the performance of organic light-emitting diodes (OLEDs), it is essential to understand and control the electric potential in the organic semiconductor layers. Electron holography (EH) is a powerful technique for visualizing the potential distribution with a transmission electron microscope. However, it has a serious issue that high-energy electrons may damage the organic layers, meaning that a low-dose EH is required. Here, we used a machine learning technique, three-dimensional (3D) tensor decomposition, to denoise electron interference patterns (holograms) of bilayer OLEDs composed of N,N'-di-[(1-naphthyl)-N,N'-diphenyl]-(1,1'-biphenyl)-4,4'-diamine (α-NPD) and tris-(8-hydroxyquinoline)aluminum (Alq3), acquired under a low-dose rate of 130 e- nm-2 s-1. The effect of denoising on the phase images reconstructed from the holograms was evaluated in terms of both the phase measurement error and the peak signal-to-noise ratio. We achieved a precision equivalent to that of a conventional measurement that had an exposure time 60 times longer. The electric field within the Alq3 layer decreased as the cumulative dose increased, which indicates that the Alq3 layer was degraded by the electron irradiation. On the basis of the degradation of the electric field, we concluded that the tolerance dose without damaging the OLED sample is about 1.7 × 105 e- nm-2, which is about 0.6 times that of the conventional EH. The combination of EH and 3D tensor decomposition denoising is capable of making a time series measurement of an OLED sample without any effect from the electron irradiation.

In the samples collected from the asteroid Ryugu, magnetite displays natural remanent magnetization due to nebular magnetic field, whereas contemporaneously grown iron sulfide does not display stable remanent magnetization. To clarify this counterintuitive feature, we observed their nanoscale magnetic domain structures using electron holography and found that framboidal magnetites have an external magnetic field of 300 A m −1 , similar to the bulk value, and its magnetic stability was enhanced by interactions with neighboring magnetites, permitting a disk magnetic field to be recorded. Micrometer-sized pyrrhotite showed a multidomain magnetic structure that was unable to retain natural remanent magnetization over a long time due to short relaxation time of magnetic-domain-wall movement, whereas submicron-sized sulfides formed a nonmagnetic phase. These results show that both magnetite and sulfide could have formed simultaneously during the aqueous alteration in the parent body of the asteroid Ryugu.

Electron holography is a useful tool for analyzing functional properties, such as electromagnetic fields and strains of materials and devices. The performance of electron holography is limited by the 'shot noise' inherent in electron micrographs (holograms), which are composed of a finite number of electrons. A promising approach for addressing this issue is to use mathematical and machine learning-based image-processing techniques for hologram denoising. With the advancement of information science, denoising methods have become capable of extracting signals that are completely buried in noise, and they are being applied to electron microscopy, including electron holography. However, these advanced denoising methods are complex and have many parameters to be tuned; therefore, it is necessary to understand their principles in depth and use them carefully. Herein, we present an overview of the principles and usage of sparse coding, the wavelet hidden Markov model and tensor decomposition, which have been applied to electron holography. We also present evaluation results for the denoising performance of these methods obtained through their application to simulated and experimentally recorded holograms. Our analysis, review and comparison of the methods clarify the impact of denoising on electron holography research.

To reduce the operating voltage, we analyzed the p–n junction of an aluminum gallium nitride (AlGaN) homojunction Tunnel Junction (TJ) deep-ultraviolet light-emitting diode using phase-shifting electron holography. We obtained a phase image reflecting the band alignment of the p–n homojunction and derived a depletion layer width of approximately 10 nm. We found the AlGaN homojunction TJ forms a p-n junction. Furthermore, the operating voltage reached 8.8 V at 63 A cm-2 by optimizing the structural characteristics of the AlGaN TJ, such as the thickness and impurity concentration, where the thickness of the TJ was 23 nm. We found that the TJ thickness should be at least the same as the depletion layer width at the AlGaN TJ.

The effectiveness of sparse coding for image inpainting and denoising of off-axis electron holograms was examined computationally based on hologram simulations according to considerations of two types of electron detectors, namely charge-coupled device (CCD) and direct-detection device (DDD) cameras. In this simulation, we used a simple-phase object with a phase step such as a semiconductor p-n junction and assumed that the holograms recorded by the CCD camera include shot noise, dark-current noise and read-out noise, while those recorded by the DDD camera include only shot noise. Simulated holograms with various electron doses were sparsely coded. Even though interference fringes cannot be recognized in the simulated CCD and DDD holograms when subjected to electron doses (per pixel) equal to 1 and 0.01, respectively, both the corresponding sparse-coded holograms exhibit meaningful interference fringes. We demonstrate that a combination of the DDD camera and sparse coding reduces the requisite dose used to obtain holograms to values less than one-thousandth compared with the CCD camera without image postprocessing. This combination is expected to generate lower-dose and/or higher-speed electron holography.

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We demonstrated the structural optimization of AlGaN tunnel junction (TJ) deep-ultraviolet light-emitting diodes by changing the thickness and impurity concentrations of p+-type and n+-type AlGaN constituting the TJ. By decreasing the total thickness of the TJ to 23 nm, the operating voltage reached a minimum of 8.8 V at 63 A cm−2. Further decrease in TJ thickness markedly increases the operating voltage. This finding implies that the depletion layer width becomes greater than the TJ thickness if it is smaller than 12 nm. Therefore, we conclude that the TJ thickness must be greater than the depletion layer width.

We analyzed the p–n junction of an aluminum gallium nitride (AlGaN) homojunction tunnel junction (TJ) deep-ultraviolet light-emitting diode by phase-shifting electron holography. We clearly obtained a phase image reflecting the band alinement of the p–n homojunction and derived a depletion layer width of approximately 10 nm. In addition, the observed depletion layer width for the AlGaN TJ was in good agreement with the simulated one reflecting the diffusion profile of Mg and Si, thus enabling a discussion on the electrical conduction mechanism for an AlGaN p–n junction.

Phase-shifting electron holography (PS-EH) is an interference transmission electron microscopy technique that accurately visualizes potential distributions in functional materials, such as semiconductors. In this paper, we briefly introduce the features of the PS-EH that overcome some of the issues facing the conventional EH based on Fourier transformation. Then, we present a high-precision PS-EH technique with multiple electron biprisms and a sample preparation technique using a cryo-focused-ion-beam, which are important techniques for the accurate phase measurement of semiconductors. We present several applications of PS-EH to demonstrate the potential in organic and inorganic semiconductors and then discuss the differences by comparing them with previous reports on the conventional EH. We show that in situ biasing PS-EH was able to observe not only electric potential distribution but also electric field and charge density at a GaAs p-n junction and clarify how local band structures, depletion layer widths and space charges changed depending on the biasing conditions. Moreover, the PS-EH clearly visualized the local potential distributions of two-dimensional electron gas layers formed at AlGaN/GaN interfaces with different Al compositions. We also report the results of our PS-EH application for organic electroluminescence multilayers and point out the significant potential changes in the layers. The proposed PS-EH enables more precise phase measurement compared to the conventional EH, and our findings introduced in this paper will contribute to the future research and development of high-performance semiconductor materials and devices.

We utilized phase-shifting electron holography on organic light emitting diodes consisting of N,N′-di-[(1-naphthyl)-N,N′-diphenyl]-(1,1′-biphenyl)-4,4′-diamine (α-NPD) and tris-(8-hydroxyquinoline)aluminum (Alq3) layers to visualize their built-in potential distribution. The bilayer showed three different electric fields, namely, the fields in the α-NPD layer, near the α-NPD/Alq3 interface, and in the Alq3 layer measured as −1.8 ± 0.4 MV m−1, −10.0 ± 2 MV m−1, 3.1 ± 0.6 MV m−1, respectively. We show that they are related to hole accumulation in the α-NPD layer, the charge carrier accumulation junction around the α-NPD/Alq3 interface, and the giant surface potential spontaneously polarized in the Alq3 layer.