In-line three-dimensional holography of nanocrystalline objects at atomic resolution

Resolution and sensitivity of the latest generation aberration-corrected transmission electron microscopes allow the vast majority of single atoms to be imaged with sub-Ångstrom resolution and their locations determined in an image plane with a precision that exceeds the 1.9-pm wavelength of 300 kV electrons. Such unprecedented performance allows expansion of electron microscopic investigations with atomic resolution into the third dimension. Here we report a general tomographic method to recover the three-dimensional shape of a crystalline particle from high-resolution images of a single projection without the need for sample rotation. The method is compatible with low dose rate electron microscopy, which improves on signal quality, while minimizing electron beam-induced structure modifications even for small particles or surfaces. We apply it to germanium, gold and magnesium oxide particles, and achieve a depth resolution of 1–2 Å, which is smaller than inter-atomic distances.

[1]  M. Malac,et al.  Radiation damage in the TEM and SEM. , 2004, Micron.

[2]  Jan Melkebeek,et al.  Stability and Dynamics , 2018 .

[3]  D. Van dyck,et al.  3D reconstruction of nanocrystalline particles from a single projection. , 2015, Micron.

[4]  V. Radmilović,et al.  3-D reconstruction of the atomic positions in a simulated gold nanocrystal based on discrete tomography: prospects of atomic resolution electron tomography. , 2008, Ultramicroscopy.

[5]  Marks,et al.  A simple channelling model for HREM contrast transfer under dynamical conditions , 1999, Journal of microscopy.

[6]  S. Pennycook,et al.  Depth sectioning with the aberration-corrected scanning transmission electron microscope. , 2006, Proceedings of the National Academy of Sciences of the United States of America.

[7]  A. Leson “There is plenty of room at the Bottom”. , 2005 .

[8]  Lin-wang Wang,et al.  Real-time sub- Å ngstrom imaging of reversible and irreversible conformations in rhodium catalysts and graphene , 2013 .

[9]  Kees Joost Batenburg,et al.  The properties of SIRT, TVM, and DART for 3D imaging of tubular domains in nanocomposite thin-films and sections. , 2014, Ultramicroscopy.

[10]  I. Ial,et al.  Nature Communications , 2010, Nature Cell Biology.

[11]  C. Jia,et al.  Determination of the 3D shape of a nanoscale crystal with atomic resolution from a single image. , 2014, Nature materials.

[12]  D. Van dyck,et al.  Do you believe that atoms stay in place when you observe them in HREM? , 2015, Micron.

[13]  David G. Barton,et al.  Quantitative Contrast Evaluation of an Industry‐Style Rhodium Nanocatalyst with Single Atom Sensitivity , 2011 .

[14]  E A Kenik,et al.  Detection of Single Atoms and Buried Defects in Three Dimensions by Aberration-Corrected Electron Microscope with 0.5-Å Information Limit , 2008, Microscopy and Microanalysis.

[15]  G. Botton,et al.  Preface. Electron-beam irradiation effects, modifications and control. , 2015, Micron.

[16]  P. Turner,et al.  Relativistic Hartree–Fock X‐ray and electron scattering factors , 1968 .

[17]  Gustaaf Van Tendeloo,et al.  Three-dimensional elemental mapping at the atomic scale in bimetallic nanocrystals. , 2013, Nano letters.

[18]  Veit Elser,et al.  Breaking the Crowther limit: combining depth-sectioning and tilt tomography for high-resolution, wide-field 3D reconstructions. , 2014, Ultramicroscopy.

[19]  John M. Gregoire,et al.  Multiphase Nanostructure of a Quinary Metal Oxide Electrocatalyst Reveals a New Direction for OER Electrocatalyst Design , 2015 .

[20]  Brian F. G. Johnson,et al.  Z-Contrast tomography: a technique inthree-dimensional nanostructural analysis based on Rutherfordscattering , 2001 .

[21]  D. Saylor,et al.  Measuring the influence of grain-boundary misorientation on thermal groove geometry in ceramic polycrystals , 2004 .

[22]  Steven G. Louie,et al.  Graphene at the Edge: Stability and Dynamics , 2009, Science.

[23]  K. H. Westmacott,et al.  PVD Growth of FCC Metal Films On Single Crystal Si And Ge Substrates , 1999 .

[24]  Fu-Rong Chen,et al.  Resolution extension and exit wave reconstruction in complex HREM. , 2004, Ultramicroscopy.

[25]  D. Van dyck,et al.  Electron channelling based crystallography. , 2007, Ultramicroscopy.

[26]  Angus I. Kirkland,et al.  Three-dimensional imaging by optical sectioning in the aberration-corrected scanning transmission electron microscope , 2009, Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences.

[27]  G. Tendeloo,et al.  Three-dimensional atomic imaging of crystalline nanoparticles , 2011, Nature.

[28]  P. Specht,et al.  Instrumental requirements for the detection of electron beam-induced object excitations at the single atom level in high-resolution transmission electron microscopy. , 2015, Micron.

[29]  A. Thust,et al.  Maximum-likelihood method for focus-variation image reconstruction in high resolution transmission electron microscopy , 1996 .

[30]  A. Credi,et al.  Bose-Einstein condensation: Where many become one and, therefore, there is plenty of room at the bottom , 2006 .

[31]  J. Miao,et al.  Electron tomography at 2.4-ångström resolution , 2012, Nature.

[32]  S. Pennycook,et al.  The possibility and implications of dynamic nanoparticle surfaces. , 2013, ACS nano.

[33]  D. Alloyeau,et al.  Atomic-resolution three-dimensional imaging of germanium self-interstitials near a surface: Aberration-corrected transmission electron microscopy , 2009 .

[34]  Jack D. Dunitz,et al.  Atomic Dispacement Parameter Nomenclature. Report of a Subcommittee on Atomic Displacement Parameter Nomenclature , 1996 .

[35]  A. Petford-Long,et al.  Dynamic Atomic-Level Rearrangements in Small Gold Particles , 1986, Science.

[36]  L. Schultz,et al.  Atomic surface diffusion on Pt nanoparticles quantified by high-resolution transmission electron microscopy. , 2014, Micron.

[37]  H. Sawada,et al.  Visualizing and identifying single atoms using electron energy-loss spectroscopy with low accelerating voltage. , 2009, Nature chemistry.

[38]  A. Kirkland,et al.  Aberration-corrected imaging of active sites on industrial catalyst nanoparticles. , 2007, Angewandte Chemie.

[39]  Fu-Rong Chen,et al.  Direct structure inversion from exit waves: Part I: Theory and simulations , 2010 .

[40]  Andrew V. Martin,et al.  Phase imaging and the evolution of a gold-vacuum interface at atomic resolution , 2006 .

[41]  Á. Barna,et al.  Amorphisation and surface morphology development at low-energy ion milling , 1998 .

[42]  Bert M. Weckhuysen,et al.  Determining the location and nearest neighbours of aluminium in zeolites with atom probe tomography , 2015, Nature Communications.

[43]  P. Sheng,et al.  Theory and Simulations , 2003 .

[44]  C. Stampfl,et al.  Shape and surface structure of gold nanoparticles under oxidizing conditions , 2008 .

[45]  Peter Schwander,et al.  An approach to quantitative high-resolution transmission electron microscopy of crystalline materials , 1995 .

[46]  Fu-Rong Chen,et al.  ‘Big Bang’ tomography as a new route to atomic-resolution electron tomography , 2012, Nature.

[47]  C. Kisielowski,et al.  3-D Reconstruction of the Atomic Positions of Defects in Simulated Gold Nanocrystals: Prospects of Atomic Resolution Electron Tomography , 2007, Microscopy and Microanalysis.

[48]  S. Pennycook,et al.  Atom-by-atom structural and chemical analysis by annular dark-field electron microscopy , 2010, Nature.