Detecting charge transfer at defects in 2D materials with electron ptychography

Author(s)
Christoph Hofer, Jacob Madsen, Toma Susi, Timothy J. Pennycook
Abstract

Electronic charge transfer at the atomic scale can reveal fundamental information about chemical bonding, but is far more challenging to directly image than the atomic structure. The charge density is dominated by the atomic nuclei, with bonding causing only a small perturbation. Thus detecting any change due to bonding requires a higher level of sensitivity than imaging structure and the overall charge density. Here we achieve the sensitivity required to detect charge transfer in both pristine and defected monolayer WS2 using the high dose efficiency of electron ptychography and its ability to correct for lens aberrations. Excellent agreement is achieved with first-principles image simulations including where thermal diffuse scattering is explicitly modelled via finite-temperature molecular dynamics based on density functional theory. The focused-probe ptychography configuration we use also provides the important ability to concurrently collect the annular dark-field signal, which can be unambiguously interpreted in terms of the atomic structure and chemical identity of the atoms, independently of the charge transfer. Our results demonstrate both the power of ptychographic reconstructions and the importance of quantitatively accurate simulations to aid their interpretation.

Organisation(s)
Physics of Nanostructured Materials
External organisation(s)
University of Antwerp
Journal
Journal of Microscopy
No. of pages
11
ISSN
0022-2720
DOI
https://doi.org/10.48550/arXiv.2301.04469
Publication date
03-2025
Peer reviewed
Yes
Austrian Fields of Science 2012
103018 Materials physics, 103043 Computational physics
Keywords
ASJC Scopus subject areas
Pathology and Forensic Medicine, Histology
Portal url
https://ucrisportal.univie.ac.at/en/publications/4abba518-febf-438e-82d0-27a03af2d56b