Atomic Images Research Articles

Ion beam assisted electron beam vacuum deposition of antireflective SiO2coating on MgAl2O4spinel

AbstractIn this paper, the electron beam vacuum coating method was used to coat a SiO2film on an MgAl2O4spinel substrate. The thickness of the coating was aimed to be 925 nm based on the physics of the antireflection coatings. Atomic force microscope images revealed that the coated silica was 880 nm thick, which is close to the aimed theoretical thickness and had 2.11 nm roughness. It could enhance the transparency of the spinel substrate by being coated on it. The infrared transmittance of the sample coated with SiO2film in the range of 3700 nm‐4800 nm was measured by a Fourier transform infrared spectrometer and reached 92.5% to 78.5%, which was about 2%–4% higher than that of MgAl2O4spinel. In addition, it was discovered that the bonding force between the coating and the substrate is determined to be about 200 MPa. The results of this study can be used for further precise design and production of antireflection coatings on the transparent materials that need more transparency.

Identification of OH groups on SrTiO3(100)-(13×13)-R33.7° reconstructed surface by non-contact atomic force microscopy and scanning tunneling microscopy

Atomic resolution imaging of a SrTiO3(100)-(13×13)-R33.7° reconstructed surface using non-contact atomic force microscopy (NC-AFM) and its simultaneous measurement with scanning tunneling microscopy (STM) is presented. Simultaneous STM and NC-AFM imaging reveals three patterns of image contrast depending on the tip apex condition and the relationship between the SrTiO3(100)-(13×13)-R33.7° surface reconstructed structure and the NC-AFM image contrast. The NC-AFM image contrast variation is deduced from the tip apex polarity on the basis of an analysis of two images with opposite contrast. This interpretation is consistent with the results of simultaneous imaging of the SrTiO3(100)-(13×13)-R33.7° surface. Furthermore, the results and interpretation identified an OH group, which is one of the surface defects, and this adsorption site.

Revealing 3D Ripple Structure and Its Dynamics in Freestanding Monolayer MoSe2 by Single-Frame 2D Atomic Image Reconstruction.

An atomic-scale ripple structure has been revealed by electron tomography based on sequential projected atomic-resolution images, but it requires harsh imaging conditions with negligible structure evolution of the imaged samples. Here, we demonstrate that the ripple structure in monolayer MoSe2 can be facilely reconstructed from a single-frame scanning transmission electron microscopy (STEM) image collected at designated collection angles. The intensity and shape of each Se2 atomic column in the single-frame projected STEM image are synergistically combined to precisely map the slight misalignments of two Se atoms induced by rippling, which is then converted to three-dimensional (3D) ripple distortions. The dynamics of 3D ripple deformation can thus be directly visualized at the atomic scale by sequential STEM imaging. In addition, the reconstructed images provide the first opportunity for directly testing the validity of the classical theory of thermal fluctuations. Our method paves the way for a 3D reconstruction of a dynamical process in two-dimensional materials with a reasonable temporal resolution.

Step‐Edge‐Induced Patterning and Orientation Control of Crystalline Organic Semiconductor Films

AbstractOrientation control over micropatterned crystalline organic semiconductor film is crucial to achieve high device performance with small variation in organic electronics. Here, using Au patterned SiO2 substrates, a method is reported to realize high‐resolution patterning and orientation control of crystalline organic thin films simultaneously. The vacuum deposited N,N‐dioctyl‐3,4,9,10‐perylene tetracarboxylic diimide (PTCDI‐C8) molecules can selectively diffuse to and nucleate on prepatterned Au stripes, resulting in patterned crystalline films with a preferential orientation distribution. Scanning tunneling microscope and high‐resolution atomic force microscope images reveal that the PTCDI‐C8 molecules first assemble on Au with perylene diimide cores in a laying down configuration, providing nucleation sites at the step edges for directional growth along the a‐axis of the molecule crystal. Subsequent deposition of molecules leads to orientated crystalline films growth due to the π packing of the perylene diimide cores, resulting in orientation control on micropatterned crystalline films. The finding provides a new strategy to grow oriented crystalline films for high device performance uniformity.

Compositionally tailored order-disorder of cation-anion sublattices in Cu2Te1-xSx solid solution thermoelectric materials

High performance thermoelectric Cu2Te1-xSx solid solutions can surprisingly be formed over a wide compositional range even with big atomic size difference between S and Te. The Cu sublattice has been found to be partially ordered and even shows amorphous substructures in some compositions, while S/Te is considered to form a chemically disordered yet crystalline sublattice. However, precise order-disorder configurations of cation-anion sublattices and their evolution upon compositional change still remain unclear. Meanwhile, the appearance of diffuse reflections on the electron diffraction patterns suggests occurrence of short-range order whose structures are not yet solved. Here, atomic structures of Cu2Te1-xSx (x = 0.1, 0.2, 0.4, 0.5, 0.6 and 0.8) have been investigated by transmission electron microscopy in both real and reciprocal spaces. The high-angle annular dark field atomic imaging indicates an approximate hexagonal stacking for S/Te atoms in all solution compositions. However, location of Cu atoms in numerous interstices of the chalcogen sublattice varies by S/Te atomic ratio, leading to change in order-disorder configurations of Cu or even nanoscale phase separation. Diffuse scattering with different geometries are identified to arise from chemical short-range order in forms of sulphur-rich atomic layers on (0001) and lath-like tellurium aggregation on {10-10}. The as-observed compositionally tailored solid solution structures and short-range order structures are found to be strongly correlated to the electron and phonon transportation in Cu2Te1-xSx. The present work indicates a promising strategy for designing solid solutions having large atomic-size mismatch which may generate abundant order/disorder atomic configurations hence greatly improve the thermoelectric properties.

Atomic Imaging of Interface Defects in an Insulating Film on Diamond.

The insulator/semiconductor interface structure is the key to electric device performance, and much interest has been focused on understanding the origin of interfacial defects. However, with conventional techniques, it is difficult to analyze the interfacial atomic structure buried in the insulating film. Here, we reveal the atomic structure at the interface between an amorphous aluminum oxide and diamond using a developed electron energy analyzer for photoelectron holography. We find that the three-dimensional atomic structure of a C-O-Al-O-C bridge between two dimer rows of the hydrogen-terminated diamond surface. Our results demonstrate that photoelectron holography can be used to reveal the three-dimensional atomic structure of the interface between a crystal and an amorphous film. We also find that the photoelectron intensity originating from the C-O bonds is strongly related to the interfacial defect density. We anticipate significant progress in the study of amorphous/crystalline interfaces based on their three-dimensional atomic structures analysis.

The effect of kink-like defects on the twin boundaries of nanotwinned Ta under nanoindentation

To figure out the effect of kink-like defects on twin boundaries, BCC Ta with three different kinds of microstructures: single crystal (SC), perfect twin boundaries (PTB) and defective twin boundaries (DTB), are studied under nanoindentation. Both indenter load and hardness in PTB are enhanced by twin boundaries but reduced in DTB due to intrinsic kink-like defects. According to atomic surface morphology, the relative sink-in depth in DTB is lower than that in PTB but higher than that in SC. By comparing atomic images of prismatic loops in three different stages, it can be found that kink-like defects in DTB perform two opposite functions: acceleration and delay. In initial plastic stage, defective twin boundaries can accelerate pinching-off event and nucleation. In transmission stage, dislocation backward emission is advanced by defective twin boundaries. In obstruction stage, the symmetry of coherent twin boundaries will be broken and asymmetrical shear loops are formed, which will delay prismatic loops moving across twin boundaries. Dislocations of 12〈111〉 are the main factor of nanoindentation in [1¯1¯2] direction. Kink-like defects will lead to less drops in DTB on dislocation densities than that in PTB. These findings are helpful to reveal the influence of intrinsic kink-like defects in BCC nanotwinned materials.

The Relevance of Building an Appropriate Environment around an Atomic Resolution Transmission Electron Microscope as Prerequisite for Reliable Quantitative Experiments: It Should Be Obvious, but It Is a Subtle Never-Ending Story!

The realization of electron microscopy facilities all over the world has experienced a paramount increase in the last decades. This means huge investments of public and private money due to the high costs of equipment, but also for maintenance and running costs. The proper design of a transmission electron microscopy facility is mandatory to fully use the advanced performances of modern equipment, capable of atomic resolution imaging and spectroscopies, and it is a prerequisite to conceive new methodologies for future advances of the knowledge. Nonetheless, even today, in too many cases around the world, the realization of the environment hosting the equipment is not appropriate and negatively influences the scientific quality of the results during the life of the infrastructure, practically vanishing the investment made. In this study, the key issues related to the realization of an advanced electron microscopy infrastructure are analyzed based on personal experience of more than thirty years, and on the literature.

Nanoscale chemical and structural investigation of solid solution polyelemental transition metal oxide nanoparticles

Although it has been shown that configurational entropy can improve the structural stability in transition metal oxides (TMOs), little is known about the oxidation state of transition metals under random mixing of alloys. Such information is essential in understanding the chemical reactivity and properties of TMOs stabilized by configurational entropy. Herein, utilizing electron energy loss spectroscopy (EELS) technique in an aberration-corrected scanning transmission electron microscope (STEM), we systematically studied the oxidation state of binary (Mn,Fe)3O4, ternary (Mn, Fe, Ni)3O4, and quinary (Mn, Fe, Ni, Cu, Zn)3O4 solid solution polyelemental transition metal oxides (SSP-TMOs) nanoparticles. Our findings show that the random mixing of multiple elements in the form of solid solution phase not only promotes the entropy stabilization but also results in stable oxidation state in transition metals spanning from binary to quinary transition metal oxide nanoparticles.

Atomic-Resolution Imaging of Micron-Sized Samples Realized by High Magnetic Field Scanning Tunneling Microscopy

Scanning tunneling microscopy (STM) can image material surfaces with atomic resolution, making it a useful tool in the areas of physics and materials. Many materials are synthesized at micron size, especially few-layer materials. Limited by their complex structure, very few STMs are capable of directly positioning and imaging a micron-sized sample with atomic resolution. Traditional STMs are designed to study the material behavior induced by temperature variation, while the physical properties induced by magnetic fields are rarely studied. In this paper, we present the design and construction of an atomic-resolution STM that can operate in a 9 T high magnetic field. More importantly, the homebuilt STM is capable of imaging micron-sized samples. The performance of the STM is demonstrated by high-quality atomic images obtained on a graphite surface, with low drift rates in the X-Y plane and Z direction. The atomic-resolution image obtained on a 32-μm graphite flake illustrates the new STM's ability of positioning and imaging micron-sized samples. Finally, we present atomic resolution images at a magnetic field range from 0 T to 9 T. The above advantages make our STM a promising tool for investigating the quantum hall effect of micron-sized layered materials.

Optimizing experimental parameters of integrated differential phase contrast (iDPC) for atomic resolution imaging

Integrated differential phase contrast scanning transmission electron microscopy (iDPC-STEM) technique has been well developed for studying atomic structures at sub-Å resolution with the capability of simultaneously imaging heavy and light atoms even at an extremely low electron dose. As a direct phase contrast imaging technique, atomic resolution iDPC-STEM is sensitive to the imaging conditions. Although great achievements have been made both in aspect of theory and experiments, the influence of experimental parameters on the contrast of atomic resolution iDPC-STEM images has not been systematically investigated. Here, we perform the iDPC-STEM simulations on the prototypical example of SrTiO3 with respect to the routine experimental factors, including the defocus, specimen thickness, accelerating voltage, convergence angle, collection angle, sample tilt and electron dose. Through the evaluation of image contrast and atom column intensity, the parameters are discussed to improve the image contrast and the visibility of light elements. Moreover, the dose-dependent simulations demonstrate the advantage of low dose iDPC-STEM imaging over other conventional STEM modes. Our results provide a practical guideline to experimentally obtain accessible atomic resolution iDPC-STEM images.

In Situ Imaging of an Anisotropic Layer-by-Layer Phase Transition in Few-Layer MoTe2

Understanding the phase transition mechanisms in two-dimensional (2D) materials is a key to precisely tailor their properties at the nanoscale. Molybdenum ditelluride (MoTe2) exhibits multiple phases at room temperature, making it a promising candidate for phase-change applications. Here, we fabricate lateral 2H-Td interfaces with laser irradiation and probe their phase transitions from micro- to atomic scales with in situ heating in the transmission electron microscope (TEM). By encapsulating the MoTe2 with graphene protection layers, we create an in situ reaction cell compatible with atomic resolution imaging. We find that the Td-to-2H phase transition initiates at phase boundaries at low temperatures (200-225 °C) and propagates anisotropically along the b-axis in a layer-by-layer fashion. We also demonstrate a fully reversible 2H-Td-2H phase transition cycle, which generates a coherent 2H lattice containing inversion domain boundaries. Our results provide insights on fabricating 2D heterophase devices with atomically sharp and coherent interfaces.

Energetic Neutral Atom Imaging of the Earth’s Ring Current and Some Results from the Chinese Double Star Program

The ring current region in the Earth’s magnetosphere contains energetic charged particles, which are injected from the magnetotail, get trapped in the inner magnetosphere, and finally drift around the Earth. The current, essentially carried by ions, is caused by the differences between the drift of the positively charged ions and that of negatively charged electrons. The charge exchange that occurs between ring current ions and geocoronal atoms determines the distribution and evolution of the ring current and lays the basis for remote detection techniques. By measuring the energetic neutral atoms produced by the charge-exchange process, the ring current can be remotely detected via energetic neutral atom imaging. The Chinese Double Star Program operated the NeUtral Atom Detector Unit (NUADU) onboard one of its two satellites for more than four years. A variety of studies were conducted using multiple methods applied to observations, such as intuitive image inspection, forward modeling, and inversion. Energetic neutral atom imaging was established as a promising technique for future imaging projects.

Investigation of microstructural development of liquid Nb in dependence of cooling rate: Molecular dynamics simulation study

In this study, the microstructural developments in the Niobium (Nb) bulk system cooled with different cooling rates from the liquid phase were investigated by the Molecular Dynamics (MD) method. The Embedded Atom Method (EAM), which includes many-body interactions, was used to calculate the interaction forces between atoms. The microstructural changes in the model system were tried to be determined by radial distribution function (RDF), voronoi polyhedra analysis (VP), determination of folded symmetries, spherical periodic order (SPO) and atomic images obtained from common neighbor analysis (CNA). Glassy structure transformations were observed for 1 × 1014 K/s, 5 × 1013 K/s, 1 × 1013 K/s cooling rates applied to the liquid Nb system, and crystal structure transformations were observed under 0 GPa pressure for 5 × 1012 K/s and 2 × 1012 K/s cooling rates. In addition, the glassy and crystalline transition temperatures at which these transformations take place were calculated. While an increase was observed in 5-fold symmetries expressing icosahedral short distance order in glassy structures obtained as a result of cooling processes, a decrease in 5-fold symmetries and an increase in 4 and 6-fold symmetries were determined in crystal structure transformations.

Deep-Learning Electron Diffractive Imaging

We report the development of deep-learning coherent electron diffractive imaging at subangstrom resolution using convolutional neural networks (CNNs) trained with only simulated data. We experimentally demonstrate this method by applying the trained CNNs to recover the phase images from electron diffraction patterns of twisted hexagonal boron nitride, monolayer graphene, and a gold nanoparticle with comparable quality to those reconstructed by a conventional ptychographic algorithm. Fourier ring correlation between the CNN and ptychographic images indicates the achievement of a resolution in the range of 0.70 and 0.55Å. We further develop CNNs to recover the probe function from the experimental data. The ability to replace iterative algorithms with CNNs and perform real-time atomic imaging from coherent diffraction patterns is expected to find applications in the physical and biological sciences.

Atomic number prior guided network for prohibited items detection from heavily cluttered X-ray imagery

Prohibited item detection in X-ray images is an effective measure to maintain public safety. Recent prohibited item detection methods based on deep learning has achieved impressive performance. Some methods improve prohibited item detection performance by introducing prior knowledge of prohibited items, such as the edge and size of an object. However, items within baggage are often placed randomly, resulting in cluttered X-ray images, which can seriously affect the correctness and effectiveness of prior knowledge. In particular, we find that different material items in X-ray images have clear distinctions according to their atomic number Z information, which is vital to suppress the interference of irrelevant background information by mining material cues. Inspired by this observation, in this paper, we combined the atomic number Z feature and proposed a novel atomic number Z Prior Guided Network (ZPGNet) to detect prohibited objects from heavily cluttered X-ray images. Specifically, we propose a Material Activation (MA) module that cross-scale flows the atomic number Z information through the network to mine material clues and reduce irrelevant information interference in detecting prohibited items. However, collecting atomic number images requires much labor, increasing costs. Therefore, we propose a method to automatically generate atomic number Z images by exploring the color information of X-ray images, which significantly reduces the manual acquisition cost. Extensive experiments demonstrate that our method can accurately and robustly detect prohibited items from heavily cluttered X-ray images. Furthermore, we extensively evaluate our method on HiXray and OPIXray, and the best result is 2.1% mAP50 higher than the state-of-the-art models on HiXray.

Thickness dependence of PbZr0.52Ti0.48O3 thin film ferroelectric parameters

Thickness is an important parameter of ferroelectric thin films, which could have a strong influence on device performance based on them. In this paper, we demonstrate the mechanism of the thickness dependence of the ferroelectric performance of a Pb(Zr0.52Ti0.48)O3 (PZT52/48) film prepared with a sol-gel method. It is observed that the spontaneous polarization (Ps) is enhanced, while the dielectric permittivity (ɛ), the coercivity field (Ec), residual polarization (Pr), efficiency (η) and energy density (Wenergy) are reduced with thicker film. In the meantime, the positive electrocaloric (EC) effect gradually transits into a negative regime. Changes in electrical properties are attributed to the increase in the tetragonal phase and the decrease in rhombohedral phase structure, due to the variation of in-plane tensile stresses with thickness which is confirmed by the atomic image of high-resolution transmission Electron microscopy. These findings provide guidance for study in modern high performance ferro-electronic device and material.

Single shot imaging for cold atoms based on machine learning

The ability to detect atoms in high spatiotemporal resolution provides a powerful tool for us to investigate the quantum properties of ultracold quantum gases. Plenty of useful imaging methods, including absorption imaging, phase contrast imaging and fluorescence imaging, have been implemented in detecting atoms. Among them, absorption imaging is the most widely used method in cold atoms laboratory. However, the traditional absorption imaging method is affected by perturbations such as interference between optical elements, fluctuation of laser power, frequency, and spatial position, resulting in residual spatially structured noise and degradation of imaging quality. Especially for regions with lower density or for longer time-of-flight, a large number of repetitions are often required to obtain better signal-to-noise ratio, which would increase the time cost and induce other noise. One must reduce the time between two imaging pulses to suppress the spatial noise. A better charge coupled device (CCD) with higher frame transfer rate or other method like fast-kinetic mode will be used to improve the imaging quality. In this paper, a single-shot cold atom imaging method based on machine learning is proposed, in which only one absorption imaging of cold atoms is required, and the corresponding background image can be generated through the neural network of an autoencoder. This effectively reduces the spatial striped noise in imaging, significantly improves the imaging quality, and makes it possible for cold atoms to be imaged multiple times in a single cycle.

2D graphitic-like gallium nitride and other structural selectivity in confinement at the graphene/SiC interface

An atomic resolution image of an intercalated structure at a graphene/SiC interface along the growth direction which is determined as a buckled GaN monolayer at the immediate interface with an underlying SiC substrate and ultrathin Ga2O3 on top.

Molecular Dynamics Simulations of Packing Structures and Local Stress in the Ge(100)/Si(110) Interface at Atomic Scale

Defects and stress distribution in the interface of Ge/Si hetero-structures play an important role in silicon-based semiconductor devices. This work at atomic scale performs molecular dynamics simulations to study the packing characteristics in the Ge/Si interface and loading features on the atoms for different contacting configurations between Ge nanopillars and Si substrates. Based on the analysis of energy, composition, the distribution of hydrostatic pressure, the Lode–Nadai parameters of each atom as well as visualized atomic packing images in the interface regions, simulation results show that contacting configurations of the Ge nanopillar with the (100) surface and the (110) surface of the Si substrate significantly affect the stability of the interface structures. The load-bearing positions of the Si surface and the inter-diffusion among the atoms in the interface regions greatly contribute to the lattice distortion of the silicon substrate, the composition, defects, and local stress distribution in the interface regions.