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

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, Alex Zettl, Narayana R. Aluru, Ramamoorthy Ramesh, Peter Ercius () and Arun Majumdar ()
Additional contact information
Joel Martis: Stanford University
Sandhya Susarla: Lawrence Berkeley National Laboratory
Archith Rayabharam: University of Illinois at Urbana-Champaign
Cong Su: University of California Berkeley
Timothy Paule: University of California Berkeley
Philipp Pelz: Lawrence Berkeley National Laboratory
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
Narayana R. Aluru: The University of Texas at Austin
Ramamoorthy Ramesh: University of California Berkeley
Peter Ercius: Lawrence Berkeley National Laboratory
Arun Majumdar: Stanford University

Nature Communications, 2023, vol. 14, issue 1, 1-8

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-39304-9

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