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

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 va...

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Main Authors: 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, Arun Majumdar
Format: Article
Language:English
Published: Nature Portfolio 2023-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-023-39304-9
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author 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
Arun Majumdar
author_facet 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
Arun Majumdar
author_sort Joel Martis
collection DOAJ
description 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.
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spelling doaj.art-4a106ab2b36f4ca59ca8339102c9b4c32023-07-23T11:19:19ZengNature PortfolioNature Communications2041-17232023-07-011411810.1038/s41467-023-39304-9Imaging the electron charge density in monolayer MoS2 at the Ångstrom scaleJoel Martis0Sandhya Susarla1Archith Rayabharam2Cong Su3Timothy Paule4Philipp Pelz5Cassandra Huff6Xintong Xu7Hao-Kun Li8Marc Jaikissoon9Victoria Chen10Eric Pop11Krishna Saraswat12Alex Zettl13Narayana R. Aluru14Ramamoorthy Ramesh15Peter Ercius16Arun Majumdar17Department of Mechanical Engineering, Stanford UniversityThe National Center for Electron Microscopy (NCEM), The Molecular Foundry, Lawrence Berkeley National LaboratoryDepartment of Mechanical Engineering, University of Illinois at Urbana-ChampaignDepartment of Physics, University of California BerkeleyDepartment of Physics, University of California BerkeleyThe National Center for Electron Microscopy (NCEM), The Molecular Foundry, Lawrence Berkeley National LaboratoryDepartment of Electrical Engineering, Stanford UniversityDepartment of Mechanical Engineering, Stanford UniversityDepartment of Mechanical Engineering, Stanford UniversityDepartment of Electrical Engineering, Stanford UniversityDepartment of Electrical Engineering, Stanford UniversityDepartment of Electrical Engineering, Stanford UniversityDepartment of Electrical Engineering, Stanford UniversityDepartment of Physics, University of California BerkeleyDepartment of Mechanical Engineering, The University of Texas at AustinDepartment of Physics, University of California BerkeleyThe National Center for Electron Microscopy (NCEM), The Molecular Foundry, Lawrence Berkeley National LaboratoryDepartment of Mechanical Engineering, Stanford UniversityAbstract 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.https://doi.org/10.1038/s41467-023-39304-9
spellingShingle 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
Arun Majumdar
Imaging the electron charge density in monolayer MoS2 at the Ångstrom scale
Nature Communications
title Imaging the electron charge density in monolayer MoS2 at the Ångstrom scale
title_full Imaging the electron charge density in monolayer MoS2 at the Ångstrom scale
title_fullStr Imaging the electron charge density in monolayer MoS2 at the Ångstrom scale
title_full_unstemmed Imaging the electron charge density in monolayer MoS2 at the Ångstrom scale
title_short Imaging the electron charge density in monolayer MoS2 at the Ångstrom scale
title_sort imaging the electron charge density in monolayer mos2 at the angstrom scale
url https://doi.org/10.1038/s41467-023-39304-9
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