Charge state-dependent symmetry breaking of atomic defects in transition metal dichalcogenides

Charge state-dependent symmetry breaking of atomic defects in transition metal dichalcogenides

Nature Communications

10.1038/s41467-024-47039-4

https://doi.org/10.1038/s41467-024-47039-4

Feifei Xiang, Lysander Huberich, Preston A. Vargas, Riccardo Torsi, Jonas Allerbeck, Anne Marie Z. Tan, Chengye Dong, Pascal Ruffieux, Roman Fasel, Oliver Gröning, Yu-Chuan Lin, Richard G. Hennig, Joshua A. Robinson, Bruno Schuler

28 March 2024

Xiang, F., Huberich, L., Vargas, P. A., Torsi, R., Allerbeck, J., Tan, A. M. Z., Dong, C., Ruffieux, P., Fasel, R., Gröning, O., Lin, Y.-C., Hennig, R. G., Robinson, J. A., & Schuler, B. (2024). Charge state-dependent symmetry breaking of atomic defects in transition metal dichalcogenides. Nature Communications, 15(1). https://doi.org/10.1038/s41467-024-47039-4

The functionality of atomic quantum emitters is intrinsically linked to their host lattice coordination. Structural distortions that spontaneously break the lattice symmetry strongly impact their optical emission properties and spin-photon interface. Here we report on the direct imaging of charge state-dependent symmetry breaking of two prototypical atomic quantum emitters in mono- and bilayer MoS2 by scanning tunneling microscopy (STM) and non-contact atomic force microscopy (nc-AFM). By changing the built-in substrate chemical potential, different charge states of sulfur vacancies (VacS) and substitutional rhenium dopants (ReMo) can be stabilized. VacS-1 as well as ReMo0 and ReMo-1 exhibit local lattice distortions and symmetry-broken defect orbitals attributed to a Jahn-Teller effect (JTE) and pseudo-JTE, respectively. By mapping the electronic and geometric structure of single point defects, we disentangle the effects of spatial averaging, charge multistability, configurational dynamics, and external perturbations that often mask the presence of local symmetry breaking.

Attribution 4.0 International (CC BY 4.0)

This research / project is supported by the Deutsche Forschungsgemeinschaft (DFG) - Walter Benjamin Program
Grant Reference no. : NA

This research / project is supported by the Swiss National Science Foundation - N/A
Grant Reference no. : 210093

This research / project is supported by the European Research Council (ERC) - European Union’s Horizon 2020 research and innovation program
Grant Reference no. : 948243

This research / project is supported by the National Institute of Standards and Technology - Semiconductor Research Corporation (SRC) program
Grant Reference no. : 70NANB17H041

This research / project is supported by the Department of Energy (DOE) - N/A
Grant Reference no. : DESC0010697

This research / project is supported by the 2D Crystal Consortium (2DCC), National Science Foundation Materials Innovation Platform - N/A
Grant Reference no. : DMR-1539916

Open Access: This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.

https://oar.a-star.edu.sg/communities-collections/articles/21429

2041-1723

Institute of High Performance Computing 

https://www.nature.com/articles/s41467-024-47039-4.pdf