查看更多>>摘要：? 2022 Elsevier B.V.High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) is a valuable method for composition determination of nanomaterials. However, light elements do not scatter efficiently into the scattering angles employed for HAADF-STEM which hinders the composition determination of material systems containing light elements by HAADF-STEM. This makes the usage of lower scattering angles favourable. Moreover, static atomic displacements (SADs) caused by the small covalent radius of the substituting light elements in semiconductor alloys increase the scattering intensity at low angles. Nevertheless, at low angles, a quantitative match between complementary image simulations and experiments is not straight forward, since e.g. inelastic scattering and correlated phonon movement is often neglected in simulations. In this study, we establish a method to quantify material systems containing light elements at low angles by resolving the remaining sources of discrepancy. An outstanding agreement between simulations and experiments is achieved by using a combination of an in-column energy filter and a fast pixelated detector. By applying this method to GaNxAs1-x quantum wells, a good agreement of the TEM results with results from high-resolution x-ray diffraction is obtained. The method developed enables the nanoscale analysis of functional materials containing light elements, especially in the presence of SADs.
查看更多>>摘要：? 2022 Elsevier B.V.De-noising is an important issue in quantitative high-resolution transmission electron microscopy (HRTEM), and its roles become even more important in applications such as beam-sensitive materials and dynamic characterisations, where the attainable signal-to-noise ratio (SNR) of HRTEM images is frequently limited. In this study, we introduce a three-dimensional stacked filter (3DSF), a novel non-linear filter in which a series of HRTEM images is stacked into a 3D data cube and then treated with the Wiener filter in the 3D domain. In comparison to the traditional Wiener filter, which is widely used for individual images, this filter can accurately estimate the power spectral density of noise and filter images with a higher SNR, fewer artefacts and greater computation efficiency, which works particularly well for HRTEM images containing periodic information and feature similarities in successive micrographs, as demonstrated by simulated and experimental images of graphene and metal–organic framework (MOF). When applied to an ultra-low dose (～8 e/?2) HRTEM image stack of MOF MIL-101, the 3DSF could distinguish 40 consecutive frames, revealing the trajectory of subtle lattice shrinkage during the exposure.
查看更多>>摘要：? 2022Correlative microscopy combines data from different microscopical techniques to gain unique insights about specimens. A key requirement to unlocking the full potential is an advanced classification method that can combine the various analytical signals into physically meaningful phases. The prevalence of highly imbalanced class distributions and high intra-class variability in such real applications makes this a difficult task, yet no study of classifier performance exists in the context of correlative microscopy. This paper investigates the application of both single classifiers as well as multiple classifier systems with dynamic selection. The test sample used for evaluation and comparison of the results is a volcanic rock where data from correlative Raman spectroscopy, Scanning Electron Microscopy (SEM) and Energy Dispersive X-ray Spectroscopy (EDS) are available and prepared for algorithmic evaluation. The results show that multiple classifier systems outperform single classifiers reaching an area under the curve of the receiver operating characteristic of 99% demonstrating the applicability of automated classification in correlative microscopy. Thus, this paper contributes by highlighting the potential of combining the research fields of correlative microscopy and machine learning.
查看更多>>摘要：? 2022 Elsevier B.V.In this second part of a series we attempt to construct an empirical model that can mimick all experimental observations made regarding the role of an alternative interleaved scan pattern in STEM imaging on the beam damage in a specific zeolite sample. We make use of a 2D diffusion model that describes the dissipation of the deposited beam energy in the sequence of probe positions that are visited during the scan pattern. The diffusion process allows for the concept of trying to ‘outrun’ the beam damage by carefully tuning the dwell time and distance between consecutively visited probe positions. We add a non linear function to include a threshold effect and evaluate the accumulated damage in each part of the image as a function of scan pattern details. Together, these ingredients are able to describe qualitatively all aspects of the experimental data and provide us with a model that could guide a further optimisation towards even lower beam damage without lowering the applied electron dose. We deliberately remain vague on what is diffusing here which avoids introducing too many sample specific details. This provides hope that the model can be applied also in sample classes that were not yet studied in such great detail by adjusting higher level parameters: a sample dependent diffusion constant and damage threshold.
查看更多>>摘要：? 2022 Elsevier B.V.Quantitative transmission electron microscopy (TEM) often requires accurate knowledge of sample thickness for determining defect density, structure factors, sample dimensions, electron beam and X-ray photons signal broadening. The most common thickness measurement is by Electron Energy Loss Spectroscopy which can be applied effectively to crystalline and amorphous materials. The drawback is that sample thickness is measured in units of Inelastic Mean Free Path (MFP) which depends on the material, the electron energy and the collection angle of the spectrometer. Furthermore, the Elastic MFP is an essential parameter for selecting optimal sample thickness to reduce dynamical scatterings, such as for short-range-order characterization of amorphous materials. Finally, the Inelastic to Elastic MFP ratio can predict the dominant mechanism for radiation damage due to the electron beam. We implement a fast and precise method for the extraction of inelastic and elastic MFP values in technologically important oxide thin films. The method relies on the crystalline Si substrate for calibration. The Inelastic MFP of Si was measured as a function of collection semi-angle (β) by combining Energy-Filtered TEM thickness maps followed by perpendicular cross-sectioning of the sample by Focused-Ion-Beam. For example, we measured a total Inelastic MFP (β～157 mrad) in Si of 145 ± 10 nm for 200 keV electrons. The MFP of the thin oxide films is determined by their ratio at their interface with Si or SiO2. The validity of this method was verified by direct TEM observation of cross-to-cross sectioning of TEM samples. The high precision of this method was enabled mainly by implementing a wedge preparation technique, which provides large sampling areas with uniform thickness. We measured the Elastic and Inelastic Mean Free Paths for 200 keV and 80 keV electrons as a function of collection angle for: SiO2 (Thermal, CVD), low-κ SiOCH, Al2O3, TiO2, ZnO, Ta2O5 and HfO2. The measured MFP values were compared to calculations based on models of Wenzel, Malis and Iakoubovskii. These models deviate from measurements by up to 30%, especially for 80 keV electrons. Hence, we propose functional relations for the Elastic MFP and Inelastic MFP in oxides with respect to the mass density and effective atomic number, which reduce deviations by a factor of 2–3. In addition, the effects of sample cooling on the measurements and sample stability are examined.
查看更多>>摘要：? 2022The noise performance and the detection limits of a direct-counting complementary metal-oxide semiconductor (CMOS) K2 camera and a charge-coupled device (CCD) camera in electron energy loss spectroscopy (EELS) experiments were evaluated. In the case of a single spectrum acquired at the shortest dwell times (2.5 ms for K2 and 1 μs for CCD), the detection limit, defined as three times the standard deviation of the spectral noise (3σ), was very low (1 e?/channel) in the counting-mode spectrum acquired with the K2 camera compared with that acquired with the CCD camera (5 e?/channel). By contrast, the spectral noise of the K2 camera changed depending on the dwell time because of the multiple read-outs related to its fixed frame rate (400 fps). The spectral noise of the K2 camera was greater than that of the CCD camera when the dwell time was longer than ～30 ms. Thus, the CCD camera was found to still be useful when detecting a very small number of electrons using a long acquisition time. In the case of an accumulated spectrum obtained by acquiring 10,000 spectra after subtracting the ultra-high-quality dark reference signal, the detection limits per read-out were ～0.016 and ～0.025 e?/channel/read-out for the K2 and CCD cameras, respectively. Because both cameras have advantages and disadvantages with respect to their detection limit, speed, and dynamic range, their proper use is important.
查看更多>>摘要：? 2022 The AuthorsDigital image comparison and matching brings many advantages over the traditional subjective human comparison, including speed and reproducibility. Despite the existence of an abundance of image difference metrics, most of them are not suited for high-resolution transmission electron microscopy (HRTEM) images. In this work we adopt two image difference metrics not widely used for TEM images. We compare them to subjective evaluation and to the mean squared error in regards to their behaviour regarding image noise pollution. Finally, the methods are applied to and tested by the task of determining precipitate sizes of a model material.
查看更多>>摘要：? 2022The effect of window material on electron beam induced phenomena in liquid phase electron microscopy (LPEM) is an interesting yet under-explored subject. We have studied the differences of electron beam induced gold nanoparticle (AuNP) growth subject to three encapsulation materials: Silicon Nitride (Si3N4), carbon and formvar. We find Si3N4 liquid cells (LCs) to result in significantly higher AuNP growth yield as compared to LCs employing the other two materials. In all cases, an electrical bias of the entire LC structures significantly affected particle growth. We demonstrate an inverse correlation of the AuNP growth rate with secondary electron (SE) emission from the windows. We attribute these differences at least in part to variations in SE emission dynamics, which is seen as a combination of material and bias dependent SE escape flux (SEEF) and SE return flux (SERF). Furthermore, our model predictions qualitatively match electrochemistry expectations.
查看更多>>摘要：? 2022 Elsevier B.V.We propose a linear imaging theory for differential phase contrast under the weak-phase-weak-amplitude object approximation. Contrast transfer functions are defined for thin and thick weak objects, and they successfully describe several imaging characteristics of differential phase contrast. We discuss the defocus dependence of the contrast for several examples: atomic resolution, a p-n junction, a heterointerface, and grain boundaries. Understanding the imaging characteristics helps in adjusting aberrations in DPC STEM.
查看更多>>摘要：? 2022We report a local mapping photoresponse of WSe2 using a second-harmonic (2w) channel based on nondestructive electrostatic force microscopy (EFM). The 2w signals resulting from interaction between WSe2 and EFM tip are intrinsically related to the electrical conductivity of WSe2. The photoresponse images and rise/decay time constants of WSe2 are obtained by local mapping 2w signals under illumination. We observe that the local photoresponse signals of WSe2 increase with the positive tip gate voltage while the WSe2 shows a p-type behavior in dark conditions We find that the reduced mobility of the photogenerated charge carriers resulting from the enhanced carrier scattering in the accumulation regime of WSe2 is responsible for the gate-dependent photoresponse behavior. Our results provide a deep understanding the intrinsic optoelectrical properties of WSe2 and contribute to the developments in the optoelectronic devices based on van der Waals layered materials.
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