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We report a method for quantitative phase recovery and simultaneous electron energy loss spectroscopy analysis using ptychographic reconstruction of a data set of "hollow" diffraction patterns. This has the potential for recovering both structural and chemical information at atomic resolution with a new generation of detectors.
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Peierls theory predicted atomic distortion in one-dimensional (1D) crystal due to its intrinsic instability in 1930. Free-standing carbon atomic chains created in situ in transmission electron microscope (TEM)1-3 are an ideal example to experimentally observe the dimerization behavior of carbon atomic chain within a finite length. We report here a surprisingly huge distortion found in the free-standing carbon atomic chains at 773 K, which is 10 times larger than the value expected in the system. Such an abnormally distorted phase only dominates at the elevated temperatures, while two distinct phases, distorted and undistorted, coexist at lower or ambient temperatures. Atom-by-atom spectroscopy indeed shows considerable variations in the carbon 1s spectra at each atomic site but commonly observes a slightly downshifted π* peak, which proves its sp1 bonding feature. These results suggest that the simple model, relaxed and straight, is not fully adequate to describe the realistic 1D structure, which is extremely sensitive to perturbations such as external force or boundary conditions.
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The edges of 2D materials show novel electronic, magnetic, and optical properties, especially when reduced to nanoribbon widths. Therefore, methods to create atomically flat edges in 2D materials are essential for future exploitation. Atomically flat edges in 2D materials are found after brittle fracture or when electrically biasing, but a simple scalable approach for creating atomically flat periodic edges in monolayer 2D transition metal dichalcogenides has yet to be realized. Here, we show how heating monolayer MoS2 to 800 °C in vacuum produces atomically flat Mo terminated zigzag edges in nanoribbons. We study this at the atomic level using an ultrastable in situ heating holder in an aberration-corrected transmission electron microscope and discriminating Mo from S at the edge, revealing unique Mo terminations for all zigzag orientations that remain stable and atomically flat when cooling back to room temperature. Highly faceted MoS2 nanoribbon constrictions are produced with Mo rich edge structures that have theoretically predicted spin separated transport channels, which are promising for spin logic applications.
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Transmission electron microscopy using low-energy electrons would be very useful for atomic resolution imaging of specimens that would be damaged at higher energies. However, the resolution at low voltages is degraded because of geometrical and chromatic aberrations. In the present study, we diminish the effect of these aberrations by using a delta-type corrector and a monochromator. The dominant residual aberration in a delta-type corrector, which is the sixth-order three-lobe aberration, is counterbalanced by other threefold aberrations. Defocus spread caused by chromatic aberration is reduced by using a monochromated beam with an energy spread of 0.05 eV. We obtain images of graphene and demonstrate atomic resolution at an ultralow accelerating voltage of 15 kV.
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Spatially resolved electron-energy-loss spectroscopy (EELS) is performed at diffuse interfaces between MoS2 and MoSe2 single layers. With a monochromated electron source (20 meV) we successfully probe excitons near the interface by obtaining the low loss spectra at the nanometer scale. The exciton maps clearly show variations even with a 10 nm separation between measurements; consequently, the optical band gap can be measured with nanometer-scale resolution, which is 50 times smaller than the wavelength of the emitted photons. By performing core-loss EELS at the same regions, we observe that variations in the excitonic signature follow the chemical composition. The exciton peaks are observed to be broader at interfaces and heterogeneous regions, possibly due to interface roughness and alloying effects. Moreover, we do not observe shifts of the exciton peak across the interface, possibly because the interface width is not much larger than the exciton Bohr radius.
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Advancements in ultrafast electron microscopy have allowed elucidation of spatially selective structural dynamics. However, as the spatial resolution and imaging capabilities have made progress, quantitative characterization of the electron pulse trains has not been reported at the same rate. In fact, inexperienced users have difficulty replicating the technique because only a few dedicated microscopes have been characterized thoroughly. Systems replacing laser driven photoexcitation with electrically driven deflectors especially suffer from a lack of quantified characterization because of the limited quantity. The primary advantages to electrically driven systems are broader frequency ranges, ease of use and simple synchronization to electrical pumping. Here, we characterize the technical parameters for electrically driven UEM including the shape, size and duration of the electron pulses using low and high frequency chopping methods. At high frequencies, pulses are generated by sweeping the electron beam across a chopping aperture. For low frequencies, the beam is continuously forced off the optic axis by a DC potential, then momentarily aligned by a countering pulse. Using both methods, we present examples that measure probe durations of 2 ns and 10 ps for the low and high frequency techniques, respectively. We also discuss how the implementation of a pulsed probe affects STEM imaging conditions by adjusting the first condenser lens.
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Enhancing the imaging power of microscopy to identify all chemical types of atom, from low- to high-atomic-number elements,would significantly contribute for a direct determination of material structures. Electron microscopes have successfully provided images of heavy-atom positions, particularly by the annular dark-field method, but detection of light atoms was difficult owing to their weak scattering power. Recent developments of aberration-correction electron optics have significantly advanced the microscope performance, enabling identification of individual light atoms such as oxygen, nitrogen, carbon, boron and lithium. However, the lightest hydrogen atom has not yet been observed directly, except in the specific condition of hydrogen adatoms on a graphene membrane. Here we show the first direct imaging of the hydrogen atom in a crystalline solid YH(2), based on a classic 'hollow-cone' illumination theory combined with state-of-the-art scanning transmission electronmicroscopy. The optimized hollow-cone condition derived from the aberration-corrected microscope parameters confirms that the information transfer can be extended to 22.5 nm(-1), which corresponds to a spatial resolution of about 44.4 pm. These experimental conditions can be readily realized with the annular bright-field imaging in scanning transmission electron microscopy according to reciprocity, revealing successfully the hydrogen-atom columns as dark dots, as anticipated from phase contrast of a weak-phase object.
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A method for measurement of the aberration status from high-resolution dark-field images is developed using scanning transmission electron microscopy (STEM), called the Segmented Image Autocorrelation function Matrix (SIAM). The method employs an autocorrelation function from the segmented area in the defocused STEM images from an aligned crystalline specimen to measure the defocus and twofold astigmatism for the probe-forming system. The values measured using this method can be fed directly back to the instrument by changing the strength of the stigmator and the objective lens of the microscope. It is successfully demonstrated that the feedback system can automatically correct the defocus and twofold astigmatism of the microscope after several iterations using practical STEM images from an actual crystalline specimen.
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Spherical aberration correctors using hexapole fields are widely used and are pivotal in atomic-resolution imaging. Although hexapole-field correctors increase the aberration-free angular range, the angular range is limited by higher-order aberrations, such as six-fold astigmatism or sixth-order three-lobe aberration. Here, we propose two types of spherical aberration correctors to compensate for geometrical aberrations up to the sixth order. The first is a four-hexapole corrector, while the second is a two-hexapole corrector, where each hexapole has a nonuniform magnetic field. The four-hexapole corrector can increase the aberration-free angle up to almost 100 mrad. The two-hexapole corrector with a nonuniform magnetic field has a smaller aberration-free angle than that of the four-hexapole corrector, but it is more compact. The dominant residual aberration in these correctors is seventh-order spherical aberration or chaplet aberration, which is seventh-order geometrical aberration.
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Annular dark-field scanning transmission electron microscope (ADF-STEM) images of an Si (001) crystal were obtained by using an aberration-corrected electron microscope, at 30-mrad convergent probe and cold field-emission gun at 300 kV. The intensity of ADF-STEM images, that is, the number of scattered electrons relative to the incident electrons, obtained for specimen thickness from 10 to 50 nm was compared quantitatively with absorptive multi-slice simulation. The column and background intensities were analyzed by column-by-column two-dimensional Gaussian fitting. These intensities were found to increase linearly with the sample thicknesses. However, the simulated image gave higher column intensity and lower background intensity for all the sample thickness. We found that experimental images were reproduced by the simulation with Gaussian convolution of 70 pm full-width at half-maximum for all the sample thicknesses from 10 to 50 nm. The possible factors accounted for this Gaussian convolution is discussed.
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Depth resolution in scanning transmission electron microscopy (STEM) is physically limited by the illumination angle. In recent notable progress on aberration correction technology, the illumination angle is significantly improved to be larger than 60 milliradians, which is 2 or 3 times larger than those in the previous generation. However, for three-dimensional depth sectioning with the large illumination angles, it is prerequisite to ultimately minimize lower orders of aberrations such as 2- and 3-fold astigmatisms and axial coma. Here, we demonstrate a live aberration correction using atomic-resolution STEM images rather than Ronchigram images. The present method could save the required time for aberration correction, and moreover, it is possible to build up a fully automated program. We demonstrate the method should be useful not only for axial depth sectioning but also phase imaging in STEM including differential phase-contrast imaging.
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Depth resolution in scanning transmission electron microscopy (STEM) is physically limited by the illumination angle. In recent notable progress on aberration correction technology, the illumination angle is significantly improved to be larger than 60 milliradians, which is 2 or 3 times larger than those in the previous generation. However, for three-dimensional depth sectioning with the large illumination angles, it is prerequisite to ultimately minimize lower orders of aberrations such as 2- and 3-fold astigmatisms and axial coma. Here, we demonstrate a live aberration correction using atomic-resolution STEM images rather than Ronchigram images. The present method could save the required time for aberration correction, and moreover, it is possible to build up a fully automated program. We demonstrate the method should be useful not only for axial depth sectioning but also phase imaging in STEM including differential phase-contrast imaging.
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Ultimate resolution in scanning transmission electron microscopy (STEM) with state-of-the-art aberration correctors requires careful tuning of the experimental parameters. The optimum aperture semi-angle depends on the chosen high tension, the chromatic aberration and the energy width of the source as well as on potentially limiting intrinsic residual aberrations. In this paper we derive simple expressions and criteria for choosing the aperture semi-angle and for counterbalancing the intrinsic sixth-order three-lobe aberration of two-hexapole aberration correctors by means of the fourth-order three-lobe aberration. It is noteworthy that for such an optimally adjusted electron probe the so-called flat area of the Ronchigram is explicitly not maximized. The above considerations are validated by experiments with a CEOS ASCOR in a C-FEG-equipped JEOL NEOARM operated at 60 kV. Sub-Angstrom resolution is demonstrated for a Si[112] single crystal as well as for a single-layered MoS2 crystalline film. Lattice reflections of 73 pm for silicon and 93 pm for molybdenum disulfide are visible in the Fourier transform of the images, respectively. Moreover, single sulfur vacancies can be clearly identified in the MoS2.
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A new area detector for atomic-resolution scanning transmission electron microscopy (STEM) is developed and tested. The circular detector is divided into 16 segments which are individually optically coupled with photomultiplier tubes. Thus, 16 atomic-resolution STEM images which are sensitive to the spatial distribution of scattered electrons on the detector plane can be simultaneously obtained. This new detector can be potentially used not only for the simultaneous formation of common bright-field, low-angle annular dark-field and high-angle annular dark-field images, but also for the quantification of images by detecting the full range of scattered electrons and even for exploring novel atomic-resolution imaging modes by post-processing combination of the individual images.
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To reduce radiation damage caused by the electron beam and to obtain high-contrast images of specimens, we have developed a highly stabilized transmission electron microscope equipped with a cold field emission gun and spherical aberration correctors for image- and probe-forming systems, which operates at lower acceleration voltages than conventional transmission electron microscopes. A delta-type aberration corrector is designed to simultaneously compensate for third-order spherical aberration and fifth-order 6-fold astigmatism. Both were successfully compensated in both scanning transmission electron microscopy (STEM) and transmission electron microscopy (TEM) modes in the range 30-60 kV. The Fourier transforms of raw high-angle annular dark field (HAADF) images of a Si[110] sample revealed spots corresponding to lattice spacings of 111 and 96 pm at 30 and 60 kV, respectively, and those of raw TEM images of an amorphous Ge film with gold particles showed spots corresponding to spacings of 91 and 79 pm at 30 and 60 kV, respectively. Er@C(82)-doped single-walled carbon nanotubes, which are carbon-based samples, were successfully observed by HAADF-STEM imaging with an atomic-level resolution.
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We visualized lithium atom columns in LiV2O4 crystals by combining scanning transmission electron microscopy with annular bright field (ABF) imaging using a spherical aberration-corrected electron microscope (R005) viewed from the [110] direction. The incident electron beam was coherent with a convergent angle of 30 mrad (semi-angle), and the detector collected scattered electrons over 20-30 mrad (semi-angle). The ABF image showed dark dots corresponding to lithium, vanadium and oxygen columns.
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Tilted illumination exit-wave restoration is compared for two aberration-corrected instruments at different accelerating voltages. The experimental progress of this technique is also reviewed and the significance of off-axial aberrations examined. Finally, the importance of higher order aberration compensation combined with careful correction of the lower order aberrations is highlighted.