The reference window for reduced perturbation of the reference wave in electrical biasing off-axis electron holography.

The perturbation of the reference wave due to electric stray fields represents a major challenge in quantitative electron holographic investigations. By introducing a focused-ion-beam-milled rectangular hole, the reference window, in an area of nearly constant electrostatic potential of the sample, this perturbation can be significantly reduced. The edge of the window forms a closed conducting loop, acting similarly to a Faraday cage, shielding the influence of the stray field on the reference wave to some extent. In this work, the shielding effect of the reference window is systematically investigated by comparing electron holograms of an electrically biased coplanar capacitor, as a well-known reference sample, with finite element simulations. It is shown that the introduction of the reference window into electrical biasing samples both suppresses unknown lateral phase distortions substantially and in addition improves the agreement of the experimentally observed phase slope with that expected by simulation significantly, particularly for small object-reference wave distances. Consequently, a slight adjustment of the sample geometry results in an improved reproducibility of electron holographic electrical biasing experiments, which is a significant step towards quantitative evaluation.

A simple and intuitive model for long-range 3D potential distributions of in-operando TEM-samples: Comparison with electron holographic tomography.

Electron holography is a powerful tool to investigate the properties of micro- and nanostructured electronic devices. A meaningful interpretation of the holographic data, however, requires an understanding of the 3D potential distribution inside and outside the sample. Standard approaches to resolve these potential distributions involve projective tilt series and their tomographic reconstruction, in addition to extensive simulations. Here, a simple and intuitive model for the approximation of such long-range potential distributions surrounding a nanostructured coplanar capacitor is presented. The model uses only independent convolutions of an initial potential distribution with a Gaussian kernel, allowing the reconstruction of the entire potential distribution from only one measured projection. By this, a significant reduction of the required computational power as well as a drastically simplified measurement process is achieved, paving the way towards quantitative electron holographic investigation of electrically biased nanostructures.

Investigation of AlGaN UV emitting tunnel junction LED devices by off-axis electron holography.

Here we use off-axis electron holography combined with advanced transmission electron microscopy techniques to understand the opto-electronic properties of AlGaN tunnel junction (TJ)-light-emitting diode (LED) devices for ultraviolet emission. Four identical AlGaN LED devices emitting at 290 nm have been grown by metal-organic chemical vapour deposition. Then Ge doped n-type regions with and without InGaN or GaN interlayers (IL) have been grown by molecular beam epitaxy onto the top Mg doped p-type layer to form a TJ and hence a high quality ohmic metal contact. Off-axis electron holography has then been used to demonstrate a reduction in the width of the TJ from 9.5 to 4.1 nm when an InGaN IL is used. As such we demonstrate that off-axis electron holography can be used to reproducibly measure nm-scale changes in electrostatic potential in highly defected and challenging materials such as AlGaN and that systematic studies of devices can be performed. The LED devices are then characterized using standard opto-electric techniques and the improvements in the performance of the LEDs are correlated with the electron holography results.

Origin of giant enhancement of phase contrast in electron holography of modulation-doped n-type GaN.

The electron optical phase contrast probed by electron holography at n-n+ GaN doping steps is found to exhibit a giant enhancement, in sharp contrast to the always smaller than expected phase contrast reported for p-n junctions. We unravel the physical origin of the giant enhancement by combining off-axis electron holography data with self-consistent electrostatic potential calculations. The predominant contribution to the phase contrast is shown to arise from the doping dependent screening length of the surface Fermi-level pinning, which is induced by FIB-implanted carbon point defects below the outer amorphous shell. The contribution of the built-in potential is negligible for modulation doping and only relevant for large built-in potentials at e.g. p-n junctions. This work provides a quantitative approach to so-called dead layers at TEM lamellas.

Measuring Electrical Resistivity at the Nanoscale in Phase-Change Materials.

Electrical resistivity is the key parameter in the active regions of many current nanoscale devices, from memristors to resistive random-access memory and phase-change memories. The local resistivity of the materials is engineered on the nanoscale to fit the performance requirements. Phase-change memories, for example, rely on materials whose electrical resistance increases dramatically with a change from a crystalline to an amorphous phase. Electrical characterization methods have been developed to measure the response of individual devices, but they cannot map the local resistance across the active area. Here, we propose a method based on operando electron holography to determine the local resistance within working devices. Upon switching the device, we show that electrical resistance is inhomogeneous on the scale of only a few nanometers.

Noise reduction of electron holography observations for a thin-foiled Nd-Fe-B specimen using the wavelet hidden Markov model.

In this study, we investigate the effectiveness of noise reduction in electron holography, based on the wavelet hidden Markov model (WHMM), which allows the reasonable separation of weak signals from noise. Electron holography observations from a Nd2Fe14B thin foil showed that the noise reduction method suppressed artificial phase discontinuities generated by phase retrieval. From the peak signal-to-noise ratio, it was seen that the impact of denoising was significant for observations with a narrow spacing of interference fringes, which is a key parameter for the spatial resolution of electron holography. These results provide essential information for improving the precision of electron holography studies.

High-precision charge analysis in a catalytic nanoparticle by electron holography.

The charge state of supported metal catalysts is the key to understand the elementary processes involved in catalytic reactions. However, high-precision charge analysis of the metal catalysts at the atomic level is experimentally challenging. To address this critical challenge, high-sensitivity electron holography has recently been successfully applied for precisely measuring the elementary charges on individual platinum nanoparticles supported on a titanium dioxide surface. In this review, we introduce the latest advancements in high-precision charge analysis and discuss the mechanisms of charge transfer at the metal-support interface. The development of charge measurements is entering a new era, and charge analyses under conditions closer to practical working environments, such as real-time, real-space, and reactive gas environments, are expected to be realized in the near future.

Measuring electrical properties in semiconductor devices by pixelated STEM and off-axis electron holography (or convergent beams vs. plane waves).

We demonstrate the use of both pixelated differential phase contrast (DPC) scanning transmission electron microscopy (STEM) and off-axis electron holography (EH) for the measurement of electric fields and assess the advantages and limitations of each technique when applied to technologically relevant samples. Three different types of samples are examined, firstly a simple highly-doped Si pn junction. Then a SiGe superlattice is examined to evaluate the effects of the mean inner potential on the measured signal. Finally, an InGaN/GaN microwire light-emitting diode (LED) device is examined which has a polarization field, variations of mean inner potential and a wurtzite crystal lattice. We discuss aspects such as spatial resolution and sensitivity, and the concept of pseudo-field is defined. However, the most important point is the need to limit the influence of diffraction contrast to obtain accurate measurements. In this respect, the use of a plane electron wave for EH is clearly beneficial when compared to the use of a convergent beam for pixelated DPC STEM.

Facilely Fabricated Zero-Bias Silicon-Based Plasmonic Photodetector in the Near-Infrared Region with a Schottky Barrier Properly Controlled by Nanoalloys.

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 ∼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.

Analysis of Nanowire pn-Junction with Combined Current-Voltage, Electron-Beam-Induced Current, Cathodoluminescence, and Electron Holography Characterization.

We present the characterization of a pn-junction GaAs nanowire. For the characterization, current-voltage, electron-beam-induced current, cathodoluminescence, and electron holography measurements are used. We show that by combining information from these four methods, in combination with drift-diffusion modelling, we obtain a detailed picture of how the nanowire pn-junction is configured and how the recombination lifetime varies axially in the nanowire. We find (i) a constant doping concentration and 600 ps recombination lifetime in the n segment at the top part of the nanowire; (ii) a 200-300 nm long gradient in the p doping next to the pn-junction; and (iii) a strong gradient in the recombination lifetime on the p side, with 600 ps lifetime at the pn-junction, which drops to 10 ps at the bottom of the p segment closest to the substrate. We recommend such complementary characterization with multiple methods for nanowire-based optoelectronic devices.

Bloch Point Quadrupole Constituting Hybrid Topological Strings Revealed with Electron Holographic Vector Field Tomography.

Topological magnetic (anti)skyrmions are robust string-like objects heralded as potential components in next-generation topological spintronics devices due to their low-energy manipulability via stimuli such as magnetic fields, heat, and electric/thermal current. While these 2D topological objects are widely studied, intrinsically 3D electron-spin real-space topology remains less explored despite its prevalence in bulky magnets. 2D-imaging studies reveal peculiar vortex-like contrast in the core regions of spin textures present in antiskyrmion-hosting thin plate magnets with S4 crystal symmetry, suggesting a more complex 3D real-space structure than the 2D model suggests. Here, holographic vector field electron tomography captures the 3D structure of antiskyrmions in a single-crystal, precision-doped (Fe0.63Ni0.3Pd0.07)3P (FNPP) lamellae at room temperature and zero field. These measurements reveal hybrid string-like solitons composed of skyrmions with topological number W = -1 on the lamellae's surfaces and an antiskyrmion (W = + 1) connecting them. High-resolution images uncover a Bloch point quadrupole (four magnetic (anti)monopoles that are undetectable in 2D imaging) which enables the observed lengthwise topological transitions. Numerical calculations corroborate the stability of hybrid strings over their conventional (anti)skyrmion counterparts. Hybrid strings result in topological tuning, a tunable topological Hall effect, and the suppression of skyrmion Hall motion, disrupting existing paradigms within spintronics.

Removal of phase residues in electron holography.

Electron holography provides quantitative phase information regarding the electromagnetic fields and the morphology of micro- to nano-scale samples. A phase image reconstructed numerically from an electron hologram sometimes includes phase residues, i.e. origins of unremovable phase discontinuities, which make it much more difficult to quantitatively analyze local phase values. We developed a method to remove the residues in a phase image by a combination of patching local areas of a hologram and denoising based on machine learning. The small patches for a hologram, which were generated using the spatial frequency information of the own fringe patterns, were pasted at each residue point by an algorithm based on sparse modeling. After successive phase reconstruction, the phase components with no dependency on the vicinity were filtered out by Gaussian process regression. We determined that the phase discontinuities that appeared around phase residues were removed and the phase distributions of an atomic resolution phase image of a Pt nanoparticle were sufficiently restored.

TEM sample preparation of lithographically patterned permalloy nanostructures on silicon nitride membranes.

We have prepared ferromagnetic nanostructures intended for the investigation of high-frequency magnetization dynamics in permalloy (Py) nanodisks using Lorentz transmission electron microscopy (LTEM) and electron holography. Py nanodisks were fabricated on thin silicon nitride (SiN) membranes using three different fabrication methods: lift-off, ion beam etching (IBE), and stencil lithography. They were further analyzed using different instruments, including scanning electron microscopy, LTEM, and electron holography. A bilayer of positive PMMA resist was utilized in the first fabrication method to form an undercut structure that guarantees a clean lift-off procedure. The second approach used dry etching with an Ar beam to etch a thin Py film, while an electron-beam-patterned negative resist mask kept the desired structure. In the third process, nanostencils (shadow masks) with submicrometer apertures were milled on SiN membranes using a focused ion beam. Furthermore, we have developed a new TEM sample preparation method, where we fabricated Py nanostructures on a bulk substrate with a SiN buffer layer and etched the substrate to create a thin SiN membrane under the Py nanostructure. Finally, we observed the vortex dynamics of the Py nanodisk under magnetic fields using LTEM and off-axis electron holography. A correlation between preparation methods and the properties of the Py nanostructures was made.

Hierarchical Fe-Co@TiO2 with Incoherent Heterointerfaces and Gradient Magnetic Domains for Electromagnetic Wave Absorption.

Induced polarization response and integrated magnetic resonance show prosperous advantages in boosting electromagnetic wave absorption but still face huge challenges in revealing the intrinsic mechanism. In this work, we propose a self-confined strategy to construct hierarchical Fe-Co@TiO2 microrods with numerous incoherent heterointerfaces and gradient magnetic domains. The results demonstrate that the use of polyvinylpyrrolidone (PVP) coating is crucial for the subsequent deposition of Co-zeolitic imidazolate frameworks (ZIF-67), the distance of ordered arranged metal ions manipulates the size of magnetic domains, and the pyrolysis of PVP layers restricts the eutectic process of Fe-Co alloys to some extent. As a result, these introduced lattice defects, oxygen vacancies, and incoherent heterointerfaces inevitably generate a strong polarization response, and the regulated gradient magnetic domains realize integrated magnetic resonance, including macroscopic magnetic coupling, long-range magnetic diffraction, and nanoscale magnetic bridge connection, and both of the intrinsic mechanisms in dissipating electromagnetic energy are quantitatively clarified by Lorentz off-axis electron holography. Owing to the cooperative merits, the Fe-Co@TiO2 absorbents exhibit enhanced absorption intensity and strong absorption bandwidth. This study inspires us to develop a generalized strategy for manipulating the size of magnetic domains, and the integrated magnetic resonance theory provides a versatile methodology in clarifying magnetic loss mechanism.

Reconstruction of Angstrom resolution exit-waves by the application of drift-corrected phase-shifting off-axis electron holography.

Phase-shifting electron holography is an excellent method to reveal electron wave phase information with very high phase sensitivity over a large range of spatial frequencies. It circumvents the limiting trade-off between fringe spacing and visibility of standard off-axis holography. Previous implementations have been limited by the independent drift of biprism and sample. We demonstrate here an advanced drift correction scheme for the hologram series that exploits the presence of an interface of the TEM specimen to the vacuum area in the hologram. It allows to obtain reliable phase information up to 2π/452 at the 1 Å information limit of the Titan 80-300 kV environmental transmission electron microscope used, by applying a moderate voltage of 250 V to a single biprism for a fringe spacing of 1 Å. The obtained phase and amplitude information is validated at a thin Pt sample by use of multislice image simulation with the frozen lattice approximation and shows excellent agreement. The presented method is applicable in any TEM equipped with at least one electron biprism and thus enables achieving high resolution off-axis holography in various instruments including those for in-situ applications. A software implementation for the acquisition, calibration and reconstruction is provided.

Room-Temperature Zero-Field kπ-Skyrmions and Their Field-Driven Evolutions in Chiral Nanodisks.

Target skyrmion, characterized by a central skyrmion surrounded by a series of concentric cylinder domains known as kπ-skyrmions (k ≥ 2), holds promise as a novel storage state in next-generation memories. However, target skyrmions comprising one or more concentric cylindrical domains have not been observed in chiral magnets, particularly at room temperature. In this study, we experimentally achieved kπ-skyrmions (k = 2, 3, and 4) with diameters of ∼220, 320, and 410 nm, respectively, and room-temperature stability under zero magnetic field by tightly confining these topological spin textures in ß-Mn-type Co8Zn10Mn2 nanodisks. The magnetic configurations and their field-driven evolutions were simultaneously investigated by using in situ off-axis electron holography. In combination with numerical simulations, we further investigated the dependence of kmax on the nanodisk diameter. These findings highlight the potential of kπ-skyrmions as information carriers and offer insights into manipulation of kπ-skyrmions in the future.

Electron holography observation of electron spin polarization around charged insulating wire.

We report direct observation by electron holography of the spin polarization of electrons in a vacuum region around a charged SiO2 wire coated with Pt-Pd. Irradiating the SiO2 wire with 300-keV electrons caused the wire to become positively charged due to the emission of secondary electrons. The spin polarization of these electrons interacting with the charged wire was observed in situ using a phase reconstruction process under an external magnetic field. The magnetic field of the spin-polarized electrons was simulated taking into account the distribution of secondary electrons and the effect of the external magnetic field.

The Mean Inner Potential of Hematite α-Fe2O3 Across the Morin Transition.

We measure the mean inner potential (MIP) of hematite, α-Fe2O3, using electron holography and transmission electron microscopy. Since the MIP is sensitive to valence electrons, we propose its use as a chemical bonding parameter for solids. Hematite can test the sensitivity of the MIP as a bonding parameter because of the Morin magnetic phase transition. Across this transition temperature, no change in the corundum crystal structure can be distinguished, while a change in hybridized Fe-3d and O-2p states was reported, affecting ionic bonding. For a given crystallographic phase, the change in the MIP with temperature is expected to be minor due to thermal expansion. Indeed, we measure the temperature dependence in corundum α-Al2O3(112¯0) between 95 and 295 K showing a constant MIP value of ∼16.8 V within the measurement accuracy of 0.45 V. Thus, our objectives are as follows: measure the MIP of hematite as a function of temperature and examine the sensitivity of the MIP as a bonding parameter for crystals. Measured MIPs of α-Fe2O3(112¯0) above the Morin transition are equal, 17.85 ± 0.50 V, 17.93 ± 0.50 V, at 295 K, 230 K, respectively. Below the Morin transition, at 95 K, a significant reduction of ∼1.3 V is measured to 16.56 ± 0.46 V. We show that this reduction follows charge redistribution resulting in increased ionic bonding.

High-Density Nanopore Confined Vortical Dipoles and Magnetic Domains on Hierarchical Macro/Meso/Micro/Nano Porous Ultra-Light Graphited Carbon for Adsorbing Electromagnetic Wave.

Atomic-level structural editing is a promising way for facile synthesis and accurately constructing dielectric/magnetic synergistic attenuated hetero-units in electromagnetic wave absorbers (EWAs), but it is hard to realize. Herein, utilizing the rapid explosive volume expansion of the CoFe-bimetallic energetic metallic triazole framework (CoFe@E-MTF) during the heat treatment, the effective absorption bandwidth and the maximum absorption intensity of a series of atomic CoFe-inserted hierarchical porous carbon (CoFe@HPC) EWAs can be modified under the diverse synthetic temperature. Under the filler loading of 15 wt%, the fully covered X and Ku bands at 3 and 2.5 mm for CoFe@HPC800 and the superb minimum reflection loss (RLmin ) of -53.15 dB and specific reflection loss (SRL) of -101.24 dB mg-1 mm-1 for CoFe@HPC1000 are achieved. More importantly, the single-atomic chemical bonding among Co─Fe on the nanopores is captured by extended X-ray absorption fine structure, which reveals the formation mechanism of nanopore-confined vortical dipoles and magnetic domains. This work heralds the infinite possibilities of atomic editing EWA in the future.

Enhancing performance of electron holography with mathematical and machine learning-based denoising techniques.

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.