Mapping valence electron distributions with multipole density formalism using 4D-STEM
Abstract
Recent advancement in aberration correction and detector technology opened a door to various applications using 4D-STEM, which yields a diffraction pattern for each scanning position within a crystal unit-cell in scanning transmission electron microscopy (STEM) and generates incredible amounts of data in momentum space. Currently 4D-STEM analysis relies on the center-of-mass of the diffraction patterns in electric field and charge density mapping. It only derives the total projected charge density and is limited to phase objects, e.g. extremely thin samples. Here, we propose a new analytical method to accurately map aspherical valence electron distributions with atom-centered multipolar functions formalism using the whole 4D-STEM dataset. We demonstrate that, with the full dynamical calculations for various sample thicknesses, the method is sensitive not only to the miniscule charge transfer, but also to the atomic site symmetry and aspherical electron orbitals. The process of the refinement is much more robust and reliable than quantitative convergent beam electron diffraction.
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1760644
- Alternate Identifier(s):
- OSTI ID: 1658413
- Report Number(s):
- BNL-220819-2021-JAAM
Journal ID: ISSN 0304-3991; TRN: US2205776
- Grant/Contract Number:
- SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Ultramicroscopy
- Additional Journal Information:
- Journal Volume: 219; Journal ID: ISSN 0304-3991
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 4D-STEM; Quantitative electron diffraction; Aberration correction; Valence electrons mapping
Citation Formats
Wu, Lijun, Meng, Qingping, and Zhu, Yimei. Mapping valence electron distributions with multipole density formalism using 4D-STEM. United States: N. p., 2020.
Web. doi:10.1016/j.ultramic.2020.113095.
Wu, Lijun, Meng, Qingping, & Zhu, Yimei. Mapping valence electron distributions with multipole density formalism using 4D-STEM. United States. https://doi.org/10.1016/j.ultramic.2020.113095
Wu, Lijun, Meng, Qingping, and Zhu, Yimei. Tue .
"Mapping valence electron distributions with multipole density formalism using 4D-STEM". United States. https://doi.org/10.1016/j.ultramic.2020.113095. https://www.osti.gov/servlets/purl/1760644.
@article{osti_1760644,
title = {Mapping valence electron distributions with multipole density formalism using 4D-STEM},
author = {Wu, Lijun and Meng, Qingping and Zhu, Yimei},
abstractNote = {Recent advancement in aberration correction and detector technology opened a door to various applications using 4D-STEM, which yields a diffraction pattern for each scanning position within a crystal unit-cell in scanning transmission electron microscopy (STEM) and generates incredible amounts of data in momentum space. Currently 4D-STEM analysis relies on the center-of-mass of the diffraction patterns in electric field and charge density mapping. It only derives the total projected charge density and is limited to phase objects, e.g. extremely thin samples. Here, we propose a new analytical method to accurately map aspherical valence electron distributions with atom-centered multipolar functions formalism using the whole 4D-STEM dataset. We demonstrate that, with the full dynamical calculations for various sample thicknesses, the method is sensitive not only to the miniscule charge transfer, but also to the atomic site symmetry and aspherical electron orbitals. The process of the refinement is much more robust and reliable than quantitative convergent beam electron diffraction.},
doi = {10.1016/j.ultramic.2020.113095},
journal = {Ultramicroscopy},
number = ,
volume = 219,
place = {United States},
year = {Tue Dec 01 00:00:00 EST 2020},
month = {Tue Dec 01 00:00:00 EST 2020}
}
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