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      Three-dimensional imaging of dislocation propagation during crystal growth and dissolution

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          Abstract

          Atomic level defects such as dislocations play key roles in determining the macroscopic properties of crystalline materials 1, 2 . Their effects range from increased chemical reactivity 3, 4 to enhanced mechanical properties 5, 6 . Dislocations have been widely studied using traditional techniques such as X-ray diffraction and optical imaging. Recent advances have enabled atomic force microscopy to study single dislocations 7 in two-dimensions (2D), while transmission electron microscopy (TEM) can now visualise strain fields in three-dimensions (3D) with near atomic resolution 810 . However, these techniques cannot offer 3D imaging of the formation or movement of dislocations during dynamic processes. Here, we describe how Bragg Coherent Diffraction Imaging (BCDI) 11, 12 can be used to visualize in 3D, the entire network of dislocations present within an individual calcite crystal during repeated growth and dissolution cycles. These investigations demonstrate the potential of BCDI for studying the mechanisms underlying the response of crystalline materials to external stimuli.

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          Most cited references30

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          Phase retrieval algorithms: a comparison

          J Fienup (1982)
          Iterative algorithms for phase retrieval from intensity data are compared to gradient search methods. Both the problem of phase retrieval from two intensity measurements (in electron microscopy or wave front sensing) and the problem of phase retrieval from a single intensity measurement plus a non-negativity constraint (in astronomy) are considered, with emphasis on the latter. It is shown that both the error-reduction algorithm for the problem of a single intensity measurement and the Gerchberg-Saxton algorithm for the problem of two intensity measurements converge. The error-reduction algorithm is also shown to be closely related to the steepest-descent method. Other algorithms, including the input-output algorithm and the conjugate-gradient method, are shown to converge in practice much faster than the error-reduction algorithm. Examples are shown.
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            Three-dimensional mapping of a deformation field inside a nanocrystal.

            Coherent X-ray diffraction imaging is a rapidly advancing form of microscopy: diffraction patterns, measured using the latest third-generation synchrotron radiation sources, can be inverted to obtain full three-dimensional images of the interior density within nanocrystals. Diffraction from an ideal crystal lattice results in an identical copy of this continuous diffraction pattern at every Bragg peak. This symmetry is broken by the presence of strain fields, which arise from the epitaxial contact forces that are inevitable whenever nanocrystals are prepared on a substrate. When strain is present, the diffraction copies at different Bragg peaks are no longer identical and contain additional information, appearing as broken local inversion symmetry about each Bragg point. Here we show that one such pattern can nevertheless be inverted to obtain a 'complex' crystal density, whose phase encodes a projection of the lattice deformation. A lead nanocrystal was crystallized in ultrahigh vacuum from a droplet on a silica substrate and equilibrated close to its melting point. A three-dimensional image of the density, obtained by inversion of the coherent X-ray diffraction, shows the expected facetted morphology, but in addition reveals a real-space phase that is consistent with the three-dimensional evolution of a deformation field arising from interfacial contact forces. Quantitative three-dimensional imaging of lattice strain on the nanometre scale will have profound consequences for our fundamental understanding of grain interactions and defects in crystalline materials. Our method of measuring and inverting diffraction patterns from nanocrystals represents a vital step towards the ultimate goal of atomic resolution single-molecule imaging that is a prominent justification for development of X-ray free-electron lasers.
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              Coherent X-ray diffraction imaging of strain at the nanoscale.

              The understanding and management of strain is of fundamental importance in the design and implementation of materials. The strain properties of nanocrystalline materials are different from those of the bulk because of the strong influence of their surfaces and interfaces, which can be used to augment their function and introduce desirable characteristics. Here we explain how new X-ray diffraction techniques, which take advantage of the latest synchrotron radiation sources, can be used to obtain quantitative three-dimensional images of strain. These methods will lead, in the near future, to new knowledge of how nanomaterials behave within active devices and on unprecedented timescales.
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                Author and article information

                Journal
                101155473
                30248
                Nat Mater
                Nat Mater
                Nature materials
                1476-1122
                21 May 2015
                01 June 2015
                August 2015
                01 February 2016
                : 14
                : 8
                : 780-784
                Affiliations
                [1 ]London Centre for Nanotechnology, University College, London WC1E 6BT, UK
                [2 ]School of Chemistry, University of Leeds, Leeds LS2 9JT, UK.
                [3 ]School of Physics and Astronomy, University of Leeds, Leeds, LS2 9JT, UK
                [4 ]Diamond Light Source, Harwell Science and Innovation Campus, Didcot, Oxon OX11 0DE, UK
                [5 ]Research Complex at Harwell, Didcot, Oxfordshire OX11 0DE, UK
                Author notes
                Correspondence and requests for materials should be addressed to jesclark@ 123456stanford.edu or F.Meldrum@ 123456leeds.ac.uk
                [†]

                Present address: Stanford PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025, USA and Center for Free-Electron Laser Science (CFEL), Deutsches Elektronensynchrotron (DESY), Notkestrasse 85, 22607 Hamburg, Germany.

                Author Contributions J.N.C. and J.I. designed the project; J.I. prepared samples; J.N.C., J.I., J.M.C., A.S.S., Y.Y.K., J.M.C., G.N. and I.K.R performed the experiments; J.N.C. performed image reconstructions; J.N.C. & I.K.R. analyzed the Data, J.N.C., J.I., F.C.M. and I.K.R. wrote the paper. All the authors read and commented on the manuscript.

                Article
                EMS63326
                10.1038/nmat4320
                4623157
                26030304
                a4ce0c9d-2241-41e0-8b87-498c00aa5fbb

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                Article

                Materials science
                calcite,calcium carbonate,imaging,coherent diffraction,screw dislocation
                Materials science
                calcite, calcium carbonate, imaging, coherent diffraction, screw dislocation

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