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      Simultaneous atomic-resolution electron ptychography and Z-contrast imaging of light and heavy elements in complex nanostructures

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          Abstract

          The aberration-corrected scanning transmission electron microscope (STEM) has emerged as a key tool for atomic resolution characterization of materials, allowing the use of imaging modes such as Z-contrast and spectroscopic mapping. The STEM has not been regarded as optimal for the phase-contrast imaging necessary for efficient imaging of light materials. Here, recent developments in fast electron detectors and data processing capability is shown to enable electron ptychography, to extend the capability of the STEM by allowing quantitative phase images to be formed simultaneously with incoherent signals. We demonstrate this capability as a practical tool for imaging complex structures containing light and heavy elements, and use it to solve the structure of a beam-sensitive carbon nanostructure. The contrast of the phase image contrast is maximized through the post-acquisition correction of lens aberrations. The compensation of defocus aberrations is also used for the measurement of three-dimensional sample information through post-acquisition optical sectioning.

          Abstract

          The use of ptychography with electrons has been limited. Here, Yang et al. demonstrate that the combination of Z-contrast and phase imaging reveals the structure of complex nanomaterials. This practical tool can be used to solve the structure of a beam-sensitive carbon nanostructure at atomic-resolution.

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          Most cited references27

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          High-resolution scanning x-ray diffraction microscopy.

          Coherent diffractive imaging (CDI) and scanning transmission x-ray microscopy (STXM) are two popular microscopy techniques that have evolved quite independently. CDI promises to reach resolutions below 10 nanometers, but the reconstruction procedures put stringent requirements on data quality and sample preparation. In contrast, STXM features straightforward data analysis, but its resolution is limited by the spot size on the specimen. We demonstrate a ptychographic imaging method that bridges the gap between CDI and STXM by measuring complete diffraction patterns at each point of a STXM scan. The high penetration power of x-rays in combination with the high spatial resolution will allow investigation of a wide range of complex mesoscopic life and material science specimens, such as embedded semiconductor devices or cellular networks.
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            The potential and limitations of neutrons, electrons and X-rays for atomic resolution microscopy of unstained biological molecules.

            Radiation damage is the main problem which prevents the determination of the structure of a single biological macromolecule at atomic resolution using any kind of microscopy. This is true whether neutrons, electrons or X-rays are used as the illumination. For neutrons, the cross-section for nuclear capture and the associated energy deposition and radiation damage could be reduced by using samples that are fully deuterated and 15N-labelled and by using fast neutrons, but single molecule biological microscopy is still not feasible. For naturally occurring biological material, electrons at present provide the most information for a given amount of radiation damage. Using phase contrast electron microscopy on biological molecules and macromolecular assemblies of approximately 10(5) molecular weight and above, there is in theory enough information present in the image to allow determination of the position and orientation of individual particles: the application of averaging methods can then be used to provide an atomic resolution structure. The images of approximately 10,000 particles are required. Below 10(5) molecular weight, some kind of crystal or other geometrically ordered aggregate is necessary to provide a sufficiently high combined molecular weight to allow for the alignment. In practice, the present quality of the best images still falls short of that attainable in theory and this means that a greater number of particles must be averaged and that the molecular weight limitation is somewhat larger than the predicted limit. For X-rays, the amount of damage per useful elastic scattering event is several hundred times greater than for electrons at all wavelengths and energies and therefore the requirements on specimen size and number of particles are correspondingly larger. Because of the lack of sufficiently bright neutron sources in the foreseeable future, electron microscopy in practice provides the greatest potential for immediate progress.
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              An improved ptychographical phase retrieval algorithm for diffractive imaging.

              The ptychographical iterative engine (or PIE) is a recently developed phase retrieval algorithm that employs a series of diffraction patterns recorded as a known illumination function is translated to a set of overlapping positions relative to a target sample. The technique has been demonstrated successfully at optical and X-ray wavelengths and has been shown to be robust to detector noise and to converge considerably faster than support-based phase retrieval methods. In this paper, the PIE is extended so that the requirement for an accurate model of the illumination function is removed.
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                Author and article information

                Journal
                Nat Commun
                Nat Commun
                Nature Communications
                Nature Publishing Group
                2041-1723
                26 August 2016
                2016
                : 7
                : 12532
                Affiliations
                [1 ]Department of Materials, University of Oxford , Parks Road, OX1 3PH Oxford, UK
                [2 ]Department of Chemistry, University of Oxford , 12 Mansfield Road, OX1 3TA Oxford, UK
                [3 ]PNDetector GmbH , Sckellstrasse 3, 81667 München, Germany
                [4 ]JEOL Ltd 3-1-2 Musashino Akishima, Tokyo 196-8558, Japan
                [5 ]PNSensor GmbH , Otto-Hahn-Ring 6, 81739 München, Germany
                [6 ]Department of Physics, University of Vienna , Boltzmanngasse 5, 1090 Vienna, Austria
                Author notes
                Article
                ncomms12532
                10.1038/ncomms12532
                5007440
                27561914
                c86f8096-3927-44ce-93db-d0481b689184
                Copyright © 2016, The Author(s)

                This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article's Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

                History
                : 22 December 2015
                : 08 July 2016
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