Surface determination through atomically resolved secondary-electron imaging
Abstract
We report that unique determination of the atomic structure of technologically relevant surfaces is often limited by both a need for homogeneous crystals and ambiguity of registration between the surface and bulk. Atomically resolved secondary-electron imaging is extremely sensitive to this registration and is compatible with faceted nanomaterials, but has not been previously utilized for surface structure determination. Here we show a detailed experimental atomic-resolution secondary-electron microscopy analysis of the c(6 x 2) reconstruction on strontium titanate (001) coupled with careful simulation of secondary-electron images, density functional theory calculations and surface monolayer-sensitive aberration-corrected plan-view high-resolution transmission electron microscopy. Our work reveals several unexpected findings, including an amended registry of the surface on the bulk and strontium atoms with unusual seven-fold coordination within a typically high surface coverage of square pyramidal TiO5 units. Lastly, dielectric screening is found to play a critical role in attenuating secondary-electron generation processes from valence orbitals.
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. of Melbourne (Australia)
- Northwestern Univ., Evanston, IL (United States)
- Hitachi High Technologies Corp., Ibaraki (Japan)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1255531
- Grant/Contract Number:
- FG02-01ER45945; DMR-1206320; AC02-05CH11231; AC02-98CH10886
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 6; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY
Citation Formats
Ciston, J., Brown, H. G., D’Alfonso, A. J., Koirala, P., Ophus, C., Lin, Y., Suzuki, Y., Inada, H., Zhu, Y., Allen, L. J., and Marks, L. D. Surface determination through atomically resolved secondary-electron imaging. United States: N. p., 2015.
Web. doi:10.1038/ncomms8358.
Ciston, J., Brown, H. G., D’Alfonso, A. J., Koirala, P., Ophus, C., Lin, Y., Suzuki, Y., Inada, H., Zhu, Y., Allen, L. J., & Marks, L. D. Surface determination through atomically resolved secondary-electron imaging. United States. https://doi.org/10.1038/ncomms8358
Ciston, J., Brown, H. G., D’Alfonso, A. J., Koirala, P., Ophus, C., Lin, Y., Suzuki, Y., Inada, H., Zhu, Y., Allen, L. J., and Marks, L. D. Wed .
"Surface determination through atomically resolved secondary-electron imaging". United States. https://doi.org/10.1038/ncomms8358. https://www.osti.gov/servlets/purl/1255531.
@article{osti_1255531,
title = {Surface determination through atomically resolved secondary-electron imaging},
author = {Ciston, J. and Brown, H. G. and D’Alfonso, A. J. and Koirala, P. and Ophus, C. and Lin, Y. and Suzuki, Y. and Inada, H. and Zhu, Y. and Allen, L. J. and Marks, L. D.},
abstractNote = {We report that unique determination of the atomic structure of technologically relevant surfaces is often limited by both a need for homogeneous crystals and ambiguity of registration between the surface and bulk. Atomically resolved secondary-electron imaging is extremely sensitive to this registration and is compatible with faceted nanomaterials, but has not been previously utilized for surface structure determination. Here we show a detailed experimental atomic-resolution secondary-electron microscopy analysis of the c(6 x 2) reconstruction on strontium titanate (001) coupled with careful simulation of secondary-electron images, density functional theory calculations and surface monolayer-sensitive aberration-corrected plan-view high-resolution transmission electron microscopy. Our work reveals several unexpected findings, including an amended registry of the surface on the bulk and strontium atoms with unusual seven-fold coordination within a typically high surface coverage of square pyramidal TiO5 units. Lastly, dielectric screening is found to play a critical role in attenuating secondary-electron generation processes from valence orbitals.},
doi = {10.1038/ncomms8358},
journal = {Nature Communications},
number = ,
volume = 6,
place = {United States},
year = {Wed Jun 17 00:00:00 EDT 2015},
month = {Wed Jun 17 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
Imaging single atoms using secondary electrons with an aberration-corrected electron microscope
journal, September 2009
- Zhu, Y.; Inada, H.; Nakamura, K.
- Nature Materials, Vol. 8, Issue 10
Image simulation for atomic resolution secondary electron image
journal, December 2012
- Wu, Lijun; Egerton, R. F.; Zhu, Yimei
- Ultramicroscopy, Vol. 123
Atomic imaging using secondary electrons in a scanning transmission electron microscope: Experimental observations and possible mechanisms
journal, June 2011
- Inada, H.; Su, D.; Egerton, R. F.
- Ultramicroscopy, Vol. 111, Issue 7
Secondary electron imaging at atomic resolution using a focused coherent electron probe
journal, February 2013
- Brown, H. G.; D'Alfonso, A. J.; Allen, L. J.
- Physical Review B, Vol. 87, Issue 5
Reconstructed Surface Structure of (111) Gold Platelets, Observed by High Resolution Techniques
journal, May 1983
- Abdelmoula, K.; Métois, J. J.; Nihoul, G.
- Physica Status Solidi (a), Vol. 77, Issue 1
High resolution images of a reconstructed surface structure on (111) gold platelets: Interpretation and comparison with theoretical models
journal, January 1983
- Nihoul, G.; Abdelmoula, K.; Métois, J. J.
- Ultramicroscopy, Vol. 12, Issue 4
High resolution surface study by In-situ UHV transmission electron microscopy
journal, January 1982
- Takayanagi, Kunio
- Ultramicroscopy, Vol. 8, Issue 1-2
Imaging the Dimers in
journal, November 1996
- Bengu, E.; Plass, R.; Marks, L. D.
- Physical Review Letters, Vol. 77, Issue 20
Atomic Structure of Si(111)- -Au from High Resolution Electron Microscopy and Heavy-Atom Holography
journal, September 1995
- Marks, L. D.; Plass, R.
- Physical Review Letters, Vol. 75, Issue 11
The structure and chemistry of the TiO2-rich surface of SrTiO3 (001)
journal, September 2002
- Erdman, Natasha; Poeppelmeier, Kenneth R.; Asta, Mark
- Nature, Vol. 419, Issue 6902
SrTiO3(001)-c(6 × 2): a long-range, atomically ordered surface stable in oxygen and ambient air
journal, November 1996
- Jiang, Qidu; Zegenhagen, Jörg
- Surface Science, Vol. 367, Issue 2
Performance and image analysis of the aberration-corrected Hitachi HD-2700C STEM
journal, March 2009
- Inada, H.; Wu, L.; Wall, J.
- Journal of Electron Microscopy, Vol. 58, Issue 3
Background, status and future of the Transmission Electron Aberration-corrected Microscope project
journal, August 2009
- Dahmen, U.; Erni, R.; Radmilovic, V.
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 367, Issue 1903, p. 3795-3808
EDM 1.0: Electron direct methods
journal, February 2005
- Kilaas, R.; Marks, L. D.; Own, C. S.
- Ultramicroscopy, Vol. 102, Issue 3
Atomic-scale structure of the reconstruction: Experiments and first-principles calculations
journal, July 2007
- Lanier, C. H.; van de Walle, A.; Erdman, N.
- Physical Review B, Vol. 76, Issue 4
Surface Structures of SrTiO 3 (001): A TiO 2 -rich Reconstruction with a c(4 × 2) Unit Cell
journal, August 2003
- Erdman, Natasha; Warschkow, Oliver; Asta, Mark
- Journal of the American Chemical Society, Vol. 125, Issue 33
Vacant-Site Octahedral Tilings on (001), the Surface, and Related Structures
journal, April 2011
- Kienzle, D. M.; Becerra-Toledo, A. E.; Marks, L. D.
- Physical Review Letters, Vol. 106, Issue 17
c(6×2) and c(4×2) reconstruction of SrTiO 3 (001)
journal, April 1999
- Jiang, Q. D.; Zegenhagen, J.
- Surface Science, Vol. 425, Issue 2-3
Formation of single-domain anatase TiO2(001)‐(1×4) islands on SrTiO3(001) after thermal annealing
journal, October 2004
- Silly, Fabien; Castell, Martin R.
- Applied Physics Letters, Vol. 85, Issue 15
Low electron energy-loss spectroscopy study of the electronic structure of matrix and Σ19, Σ13 boundaries in SrTiO 3
journal, January 2005
- Hu, K. X.; Jones, I. P.
- Journal of Physics D: Applied Physics, Vol. 38, Issue 2
Synthesis-Dependent Atomic Surface Structures of Oxide Nanoparticles
journal, October 2013
- Lin, Yuyuan; Wen, Jianguo; Hu, Linhua
- Physical Review Letters, Vol. 111, Issue 15
The chemical bond and atomic displacements in SrTiO3 from X-ray diffraction analysis
journal, December 1995
- Abramov, Yu. A.; Tsirelson, V. G.; Zavodnik, V. E.
- Acta Crystallographica Section B Structural Science, Vol. 51, Issue 6
Charge density distributions of strontium titanate obtained by the maximum entropy method
journal, May 1998
- Ikeda, T.
- Solid State Ionics, Vol. 108, Issue 1-4
Electron-density distribution in cubic SrTiO 3 : a comparative γ-ray diffraction study
journal, June 2005
- Jauch, W.; Reehuis, M.
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 61, Issue 4
Experimental surface charge density of the surface
journal, August 2006
- Ciston, J.; Marks, L. D.; Feidenhans’l, R.
- Physical Review B, Vol. 74, Issue 8
Diffraction refinement of localized antibonding at the Si(111) surface
journal, May 2009
- Ciston, J.; Subramanian, A.; Robinson, I. K.
- Physical Review B, Vol. 79, Issue 19
Concentric-shell algorithm for Auger and core-level photoelectron diffraction: Theory and applications
journal, September 1993
- Saldin, D. K.; Harp, G. R.; Chen, X.
- Physical Review B, Vol. 48, Issue 11
Mapping energy bands in layer compounds from the angular dependence of ultraviolet photoemission
journal, July 1974
- Smith, Neville V.; Traum, Morton M.; Di Salvo, F. J.
- Solid State Communications, Vol. 15, Issue 2
Secondary electron emission from tungsten. Observation of the electronic structure of the semi-infinite crystal
journal, January 1979
- Christensen, N. Egede; Willis, R. F.
- Journal of Physics C: Solid State Physics, Vol. 12, Issue 1
Secondary-electron-emission spectroscopy of tungsten: Angular dependence and phenomenology
journal, November 1978
- Willis, Roy F.; Christensen, Niels Egede
- Physical Review B, Vol. 18, Issue 10
Electron scattering by atomic hydrogen: Elastic and inelastic phenomena at 13.9–200 eV
journal, November 1991
- Bray, Igor; Konovalov, Dmitry A.; McCarthy, Ian E.
- Physical Review A, Vol. 44, Issue 9
Electron scattering by atomic sodium: 3 S –3 and 3 S –3 P cross sections at 10 to 100 eV
journal, December 1991
- Bray, Igor; Konovalov, Dmitry A.; McCarthy, Ian E.
- Physical Review A, Vol. 44, Issue 11
Low-energy elastic scattering of electrons from atomic oxygen
journal, November 1989
- Williams, J. F.; Allen, L. J.
- Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 22, Issue 21
Quantitative electron spectroscopy of surfaces: A standard data base for electron inelastic mean free paths in solids
journal, February 1979
- Seah, M. P.; Dench, W. A.
- Surface and Interface Analysis, Vol. 1, Issue 1
Determination of the complex dielectric function of epitaxial SrTiO3 films using transmission electron energy-loss spectroscopy
journal, March 1999
- Ryen, L.; Wang, X.; Helmersson, U.
- Journal of Applied Physics, Vol. 85, Issue 5
Theory of dielectric screening and electron energy loss spectroscopy at surfaces
journal, July 2009
- Hogan, Conor; Palummo, Maurizia; Del Sole, Rodolfo
- Comptes Rendus Physique, Vol. 10, Issue 6
Theory and Application for the Scanning Tunneling Microscope
journal, June 1983
- Tersoff, J.; Hamann, D. R.
- Physical Review Letters, Vol. 50, Issue 25
Fixed-Point Optimization of Atoms and Density in DFT
journal, May 2013
- Marks, L. D.
- Journal of Chemical Theory and Computation, Vol. 9, Issue 6
Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces
journal, April 2008
- Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I.
- Physical Review Letters, Vol. 100, Issue 13
Comparative assessment of a new nonempirical density functional: Molecules and hydrogen-bonded complexes
journal, December 2003
- Staroverov, Viktor N.; Scuseria, Gustavo E.; Tao, Jianmin
- The Journal of Chemical Physics, Vol. 119, Issue 23
High resolution surface study by In-situ UHV transmission electron microscopy
journal, January 1982
- Takayanagi, Kunio
- Ultramicroscopy, Vol. 8, Issue 1-2
Single atom imaging in high-resolution UHV electron microscopy: Bi on Si(111) surface
journal, August 1992
- Haga, Y.; Takayanagi, K.
- Ultramicroscopy, Vol. 45, Issue 1
Theory of dielectric screening and electron energy loss spectroscopy at surfaces
journal, July 2009
- Hogan, Conor; Palummo, Maurizia; Del Sole, Rodolfo
- Comptes Rendus Physique, Vol. 10, Issue 6
EDM 1.0: Electron direct methods
journal, February 2005
- Kilaas, R.; Marks, L. D.; Own, C. S.
- Ultramicroscopy, Vol. 102, Issue 3
Image simulation for atomic resolution secondary electron image
journal, December 2012
- Wu, Lijun; Egerton, R. F.; Zhu, Yimei
- Ultramicroscopy, Vol. 123
Surface Structures of SrTiO 3 (001): A TiO 2 -rich Reconstruction with a c(4 × 2) Unit Cell
journal, August 2003
- Erdman, Natasha; Warschkow, Oliver; Asta, Mark
- Journal of the American Chemical Society, Vol. 125, Issue 33
Background, status and future of the Transmission Electron Aberration-corrected Microscope project
journal, August 2009
- Dahmen, U.; Erni, R.; Radmilovic, V.
- Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 367, Issue 1903, p. 3795-3808
Retarded field calculation of electron energy loss in inhomogeneous dielectrics
journal, March 2002
- García de Abajo, F. J.; Howie, A.
- Physical Review B, Vol. 65, Issue 11
Water-driven structural evolution of the polar MgO (111) surface: An integrated experimental and theoretical approach
journal, February 2009
- Ciston, J.; Subramanian, A.; Marks, L. D.
- Physical Review B, Vol. 79, Issue 8
Theory of Angular Resolved Photoemission from Adsorbates
journal, May 1974
- Liebsch, A.
- Physical Review Letters, Vol. 32, Issue 21
Extinction-free electron diffraction refinement of bonding in SrTiO 3
journal, August 2004
- Friis, Jesper; Jiang, Bin; Spence, John
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 60, Issue 5
Electron density and energy density view on the atomic interactions in SrTiO 3
journal, July 2002
- Zhurova, Elizabeth A.; Tsirelson, Vladimir G.
- Acta Crystallographica Section B Structural Science, Vol. 58, Issue 4
Atomic Imaging Using Secondary Electrons in a Scanning Transmission Electron Microscope : Experimental Observations and Possible Mechanisms
preprint, January 2010
- Inada, H.; Su, D.; Egerton, R. F.
- arXiv
Works referencing / citing this record:
Simultaneous atomic-resolution electron ptychography and Z-contrast imaging of light and heavy elements in complex nanostructures
journal, August 2016
- Yang, H.; Rutte, R. N.; Jones, L.
- Nature Communications, Vol. 7, Issue 1
Nanoparticle shape, thermodynamics and kinetics
journal, January 2016
- Marks, L. D.; Peng, L.
- Journal of Physics: Condensed Matter, Vol. 28, Issue 5
Surface-screening mechanisms in ferroelectric thin films and their effect on polarization dynamics and domain structures
journal, January 2018
- Kalinin, Sergei V.; Kim, Yunseok; Fong, Dillon D.
- Reports on Progress in Physics, Vol. 81, Issue 3
Exact Time-Dependent Exchange-Correlation Potential in Electron Scattering Processes
journal, December 2017
- Suzuki, Yasumitsu; Lacombe, Lionel; Watanabe, Kazuyuki
- Physical Review Letters, Vol. 119, Issue 26
How heteroepitaxy occurs on strontium titanate
journal, April 2019
- Cook, Seyoung; Letchworth-Weaver, Kendra; Tung, I-Cheng
- Science Advances, Vol. 5, Issue 4