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Imaging the electron charge density in monolayer MoS2 at the Ångstrom scale

Author

Listed:
  • Joel Martis

    (Stanford University)

  • Sandhya Susarla

    (Lawrence Berkeley National Laboratory
    Lawrence Berkeley National Laboratory
    Arizona State University)

  • Archith Rayabharam

    (University of Illinois at Urbana-Champaign)

  • Cong Su

    (University of California Berkeley
    University of California Berkeley
    Kavli Energy NanoScience Institute, University of California Berkeley)

  • Timothy Paule

    (University of California Berkeley
    University of California Berkeley
    Kavli Energy NanoScience Institute, University of California Berkeley)

  • Philipp Pelz

    (Lawrence Berkeley National Laboratory
    Institute of Micro- and Nanostructure Research & Center for Nanoanalysis and Electron Microscopy (CENEM), Department of Materials Science, Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU))

  • Cassandra Huff

    (Stanford University)

  • Xintong Xu

    (Stanford University)

  • Hao-Kun Li

    (Stanford University)

  • Marc Jaikissoon

    (Stanford University)

  • Victoria Chen

    (Stanford University)

  • Eric Pop

    (Stanford University)

  • Krishna Saraswat

    (Stanford University)

  • Alex Zettl

    (University of California Berkeley
    University of California Berkeley
    Kavli Energy NanoScience Institute, University of California Berkeley)

  • Narayana R. Aluru

    (The University of Texas at Austin)

  • Ramamoorthy Ramesh

    (University of California Berkeley
    University of California Berkeley)

  • Peter Ercius

    (Lawrence Berkeley National Laboratory)

  • Arun Majumdar

    (Stanford University)

Abstract

Four-dimensional scanning transmission electron microscopy (4D-STEM) has recently gained widespread attention for its ability to image atomic electric fields with sub-Ångstrom spatial resolution. These electric field maps represent the integrated effect of the nucleus, core electrons and valence electrons, and separating their contributions is non-trivial. In this paper, we utilized simultaneously acquired 4D-STEM center of mass (CoM) images and annular dark field (ADF) images to determine the projected electron charge density in monolayer MoS2. We evaluate the contributions of both the core electrons and the valence electrons to the derived electron charge density; however, due to blurring by the probe shape, the valence electron contribution forms a nearly featureless background while most of the spatial modulation comes from the core electrons. Our findings highlight the importance of probe shape in interpreting charge densities derived from 4D-STEM and the need for smaller electron probes.

Suggested Citation

  • Joel Martis & Sandhya Susarla & Archith Rayabharam & Cong Su & Timothy Paule & Philipp Pelz & Cassandra Huff & Xintong Xu & Hao-Kun Li & Marc Jaikissoon & Victoria Chen & Eric Pop & Krishna Saraswat &, 2023. "Imaging the electron charge density in monolayer MoS2 at the Ångstrom scale," Nature Communications, Nature, vol. 14(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39304-9
    DOI: 10.1038/s41467-023-39304-9
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    References listed on IDEAS

    as
    1. Yi Jiang & Zhen Chen & Yimo Han & Pratiti Deb & Hui Gao & Saien Xie & Prafull Purohit & Mark W. Tate & Jiwoong Park & Sol M. Gruner & Veit Elser & David A. Muller, 2018. "Electron ptychography of 2D materials to deep sub-ångström resolution," Nature, Nature, vol. 559(7714), pages 343-349, July.
    2. Timm Bredtmann & Misha Ivanov & Gopal Dixit, 2014. "X-ray imaging of chemically active valence electrons during a pericyclic reaction," Nature Communications, Nature, vol. 5(1), pages 1-7, December.
    3. Knut Müller & Florian F. Krause & Armand Béché & Marco Schowalter & Vincent Galioit & Stefan Löffler & Johan Verbeeck & Josef Zweck & Peter Schattschneider & Andreas Rosenauer, 2014. "Atomic electric fields revealed by a quantum mechanical approach to electron picodiffraction," Nature Communications, Nature, vol. 5(1), pages 1-8, December.
    4. Shiang Fang & Yi Wen & Christopher S. Allen & Colin Ophus & Grace G. D. Han & Angus I. Kirkland & Efthimios Kaxiras & Jamie H. Warner, 2019. "Atomic electrostatic maps of 1D channels in 2D semiconductors using 4D scanning transmission electron microscopy," Nature Communications, Nature, vol. 10(1), pages 1-9, December.
    5. Zhen Chen & Michal Odstrcil & Yi Jiang & Yimo Han & Ming-Hui Chiu & Lain-Jong Li & David A. Muller, 2020. "Mixed-state electron ptychography enables sub-angstrom resolution imaging with picometer precision at low dose," Nature Communications, Nature, vol. 11(1), pages 1-10, December.
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