Disorder-tuned conductivity in amorphous monolayer carbon.

Correlating atomic configurations-specifically, degree of disorder (DOD)-of an amorphous solid with properties is a long-standing riddle in materials science and condensed matter physics, owing to difficulties in determining precise atomic positions in 3D structures1-5. To this end, 2D systems provide insight to the puzzle by allowing straightforward imaging of all atoms6,7. Direct imaging of amorphous monolayer carbon (AMC) grown by laser-assisted depositions has resolved atomic configurations, supporting the modern crystallite view of vitreous solids over random network theory8. Nevertheless, a causal link between atomic-scale structures and macroscopic properties remains elusive. Here we report facile tuning of DOD and electrical conductivity in AMC films by varying growth temperatures. Specifically, the pyrolysis threshold temperature is the key to growing variable-range-hopping conductive AMC with medium-range order (MRO), whereas increasing the temperature by 25 °C results in AMC losing MRO and becoming electrically insulating, with an increase in sheet resistance of 109 times. Beyond visualizing highly distorted nanocrystallites embedded in a continuous random network, atomic-resolution electron microscopy shows the absence/presence of MRO and temperature-dependent densities of nanocrystallites, two order parameters proposed to fully describe DOD. Numerical calculations establish the conductivity diagram as a function of these two parameters, directly linking microstructures to electrical properties. Our work represents an important step towards understanding the structure-property relationship of amorphous materials at the fundamental level and paves the way to electronic devices using 2D amorphous materials.

Aberration Correction for Large-Angle Illumination Scanning Transmission Electron Microscopy by Using Iterative Electron Ptychography Algorithms.

Modern aberration correctors in the scanning transmission electron microscope (STEM) have dramatically improved the attainable spatial resolution and enabled atomical structure and spectroscopic analysis even at low acceleration voltages (≤80 kV). For a large-angle illumination, achieving successful aberration correction to high angles is challenging with an aberration corrector, which limits further improvements in applications such as super-resolution, three-dimensional atomic depth resolution, or atomic surface morphology analyses. Electron ptychography based on four-dimensional STEM can provide a postprocessing strategy to overcome the current technological limitations. In this work, we have demonstrated that aberration correction for large-angle illumination is feasible by pushing the capabilities of regularized ptychographic iterative engine algorithms to reconstruct 4D data sets acquired using a relatively low-efficiency complementary metal oxide semiconductor camera. We report super resolution (0.71 Å) with large-angle illumination (50-60 mrad) and under 60 kV accelerating voltage.

Simultaneous three-dimensional deformation measurement using tri-wavelength and monochrome camera imaging with a pyramid prism.

What we believe to be a new electronic speckle pattern interferometry (ESPI) configuration is being developed for simultaneous three-dimensional deformation measurements. In this ESPI system, two pairs of symmetrical illuminating arrangement with dual-wavelength lights were used to independently sense two in-plane deformation components, one Michelson interferometer-based set illuminating with the other wavelength light was utilized to measure out-of-plane deformation. The color speckle interferogram was split into four sub-patterns by a prism, three of them were filtered by three different bandpass dichroic filters and recorded by one monochrome camera. Micro-rotation testing work firstly verifies the validation of the proposed phase-shifting device. Three-dimensional deformation information was simultaneous obtained by using temporal phase-shift method. All strain components related to the specimen surface deformation were further determined by numerical differential. The experimental results of a tested specimen were excellently consistent with those of FEM simulation, which verified the validation and feasibility of the proposed ESPI system for measuring 3D deformation.

Measurement of natural frequencies and mode shapes of transparent insect wings using common-path ESPI.

In this study, a common-path electronic speckle pattern interferometry system which upholds the natural property of transparency of insect's wings has been developed to measure the wings' natural frequencies and mode shapes for the first time. A novel base-exciting method was designed to enable the simultaneous application of sinusoidal and static forces to excite wings and introduce an additional phase. The moiré effect induced by the amplitude modulation was employed to accurately recognize the resonance state. Subsequently, the mode shapes were visualized by phase-shifting and real-time frame subtraction. Eight pairs of forewings from cicadas were investigated. The first three order natural frequencies of the wings are approximately 145 Hz, 272 Hz and 394 Hz, respectively, which are dispersed to prevent modal coupling. The cambered mode shapes exhibit a strongly spanwise-chordwise anisotropy flexural stiffness distribution, generally dominated by bending and twisting deformation. The details of the high-order mode shapes show that the tip exhibits distinct deformation, indicating more flexibility to cope with external impact load, and the nodal lines usually comply with the direction of the wing veins in higher modes, substantiating the fact that the veins play an important role as stiffeners of the membrane. The results are in excellent agreement with the dynamic performance of previous studies, which will potentially affect a broader community of optical measurement specialists and entomologists to enhance our understanding of time-averaged interferograms and insect flights.

Experimental verification of full-field accuracy in stereo-DIC based on the ESPI method.

This paper proposes a method to merge stereo-digital image correlation (DIC) and electronic speckle pattern interferometry (ESPI) data by camera calibration. The proposed method is employed to verify the accuracy of full-field out-of-plate displacements measured by stereo-DIC in a cantilever beam test. The mean absolute error and the root mean square error (RMSE) of the full-field displacement measured by four-megapixel cameras are 0.849 µm and 1.08 µm at 60 mm field of view, respectively, and the RMSE of the central area is 0.615 µm. The errors are not uniformly distributed because of the imperfect calibration. When the lenses are changed and the field of view reaches 120 mm, the RMSE is 1.48 µm with uniform distribution. These accuracies could be traced back to the laser wavelength to confirm the stereo-DIC data. The proposed method can be used not only to verify the full-field measurement accuracy of DIC but also to determine the rigid-body displacement for ESPI with a high-precision stereo-DIC. Thus, the displacement vector can be obtained. Furthermore, it can unify the coordinate of multiple ESPI systems to achieve a large range of high-precision three-dimensional deformation measurements.

Accurate and Robust Calibration of the Uniform Affine Transformation Between Scan-Camera Coordinates for Atom-Resolved In-Focus 4D-STEM Datasets.

Accurate geometrical calibration between the scan coordinates and the camera coordinates is critical in four-dimensional scanning transmission electron microscopy (4D-STEM) for both quantitative imaging and ptychographic reconstructions. For atomic-resolved, in-focus 4D-STEM datasets, we propose a hybrid method incorporating two sub-routines, namely a J-matrix method and a Fourier method, which can calibrate the uniform affine transformation between the scan-camera coordinates using raw data, without a priori knowledge of the crystal structure of the specimen. The hybrid method is found robust against scan distortions and residual probe aberrations. It is also effective even when defects are present in the specimen, or the specimen becomes relatively thick. We will demonstrate that a successful geometrical calibration with the hybrid method will lead to a more reliable recovery of both the specimen and the electron probe in a ptychographic reconstruction. We will also show that, although the elimination of local scan position errors still requires an iterative approach, the rate of convergence can be improved, and the residual errors can be further reduced if the hybrid method can be firstly applied for initial calibration. The code is made available as a simple-to-use tool to correct affine transformations of the scan-camera coordinates in 4D-STEM experiments.

Efficient ESPI method to identify vibration characteristics of transparent films.

Electronic speckle pattern interferometry (ESPI) has been frequently used to study vibration characteristics of engineering structures. However, efficient ESPI methods for identifying the vibration characteristics of transparent membranes are rarely reported. A convenient approach to determine the resonant frequencies and the vibration modes of transparent films is proposed. A quasi-common-path ESPI (QCP-ESPI) is developed to detect out-of-plane deformation and visualize vibrational modes of a vibrating transparent diaphragm. An amplitude-modulation-based method is proposed for quick and accurate determining resonance of oscillating objects during frequency scanning. Experimental performances demonstrate the feasibility and efficiency of the QCP-ESPI and amplitude-modulation-based methods for determining the resonant frequency and vibration modes of transparent objects.

Panoramic dual-directional shearography assisted by a bi-mirror.

A panoramic dual-directional shearography system is proposed to simultaneously determine out-of-plane deformation derivatives in two directions and globally inspect the object to be tested. A dichroic filter (DF), a 3CCD camera, and dual-wavelength light are used in the proposed shearography configuration. The dual-wavelength light coupled with the corresponding imaging sensors of the 3CCD camera provides independent color signals and shearograms. Through adjustment of the tilted stereo-angle of the DF, which offers a second wavelength-dependent measurement, an additional independent image-shearing can be introduced into the setup. The auxiliary bi-mirror surrounding the object helps to fully illuminate the object surface and capture it in a single shot. Theoretical analysis and experimental results demonstrated the utility of the system.

Degree of disorder-regulated ion transport through amorphous monolayer carbon.

Nanopore technology, re-fueled by two-dimensional (2D) materials such as graphene and MoS2, controls mass transport by allowing certain species while denying others at the nanoscale and has a wide application range in DNA sequencing, nano-power generation, and others. With their low transmembrane transport resistance and high permeability stemming from their ultrathin nature, crystalline 2D materials do not possess nanoscale holes naturally, thus requiring additional fabrication to create nanopores. Herein, we demonstrate that nanopores exist in amorphous monolayer carbon (AMC) grown at low temperatures. The size and density of nanopores can be tuned by the growth temperature, which was experimentally verified by atomic images and further corroborated by kinetic Monte Carlo simulation. Furthermore, AMC films with varied degrees of disorder (DOD) exhibit tunable transmembrane ionic conductance over two orders of magnitude when serving as nanopore membranes. This work demonstrates the DOD-tuned property in amorphous monolayer carbon and provides a new candidate for modern membrane science and technology.

Collective Magnetic Behavior in Vanadium Telluride Induced by Self-Intercalation.

Self-intercalation of native magnetic atoms within the van der Waals (vdW) gap of layered two-dimensional (2D) materials provides a degree of freedom to manipulate magnetism in low-dimensional systems. Among various vdW magnets, the vanadium telluride is an interesting system to explore the interlayer order-disorder transition of magnetic impurities due to its flexibility in taking nonstoichiometric compositions. In this work, we combine high-resolution scanning transmission electron microscopy (STEM) analysis with density functional theory (DFT) calculations and magnetometry measurements, to unveil the local atomic structure and magnetic behavior of V-rich V1+xTe2 nanoplates with embedded V3Te4 nanoclusters grown by chemical vapor deposition (CVD). The segregation of V intercalations locally stabilizes the self-intercalated V3Te4 magnetic phase, which possesses a distorted 1T'-like monoclinic structure. This phase transition is controlled by the electron doping from the intercalant V ions. The magnetic hysteresis loops show that the nanoplates exhibit superparamagnetism, while the temperature-dependent magnetization curves evidence a collective superspin-glass magnetic behavior of the nanoclusters at low temperature. Using four-dimensional (4D) STEM diffraction imaging, we reveal the formation of collective diffuse magnetic domain structures within the sample under the high magnetic fields inside the electron microscope. Our results shed light on the studies of dilute magnetism at the 2D limit and on strategies for the manipulation of magnetism for spintronic applications.

Anisotropic point defects in rhenium diselenide monolayers.

Point defects in 1T″ anisotropic ReSe2 offer many possibilities for defect engineering, which could endow this two-dimensional semiconductor with new functionalities, but have so far received limited attention. Here, we systematically investigate a full spectrum of point defects in ReSe2, including vacancies (VSe1-4), isoelectronic substitutions (OSe1-4 and SSe1-4), and antisite defects (SeRe1-2 and ReSe1-4), by atomic-scale electron microscopy imaging and density functional theory (DFT) calculations. Statistical counting reveals a diverse density of various point defects, which are further elaborated by the formation energy calculations. Se vacancy dynamics was unraveled by in-situ electron beam irradiation. DFT calculations reveal that vacancies at Se sites notably introduce in-gap states, which are largely quenched upon isoelectronic substitutions (O and S), whereas antisite defects introduce localized magnetic moments. These results provide atomic-scale insight of atomic defects in 1T″-ReSe2, paving the way for tuning the electronic structure of anisotropic ReSe2 via defect engineering.

Designed for the enhancement of structure mechanostability and strength: Suture-serrate margins of bivalve shells.

Through biological evolution, bivalve mollusks developed shells to improve the utilization of metabolic energy and provide protection against external threats. In addition to the mechanical optimization of the microstructure, the design of the macroscopic shape of a bivalve shell naturally becomes a potential approach to achieving the aforementioned purposes. While the functions of some features of mollusk shells have been studied, the role of the suture-serrate margins, a common morphology of bivalve shell edges, in the global mechanical behaviors of bivalve shells requires further exploration. Here, we present how the serrate margins contribute to the global mechanical properties of bivalve shells. The results of the compression tests employed on a typical bivalve, M. mercenaria, showed that the complete bivalve shells with suture-serrate margins perform better in terms of strength and work to fracture than those without the margins under the same conditions (dry and wet). The primary failure types observed during compression reveal that the failure mechanisms of valve shells are dependent on the suture-serrate margin morphology and water content. Using numerical simulations, the mechanical functions of the suture-serrate margins were demonstrated. Specifically, serrate margins provide mutual resistance by "locking" complementary valves to redistribute and eliminate stress concentrations around pre-existing defects, thereby enhancing the mechanostability and strength of the entire structure.