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

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

doi:10.1038/s41467-024-47039-4

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

Nat Commun. 2024 Mar 28;15(1):2738. doi: 10.1038/s41467-024-47039-4.

Authors

Feifei Xiang^#¹, Lysander Huberich^#¹, Preston A Vargas^#², Riccardo Torsi³, Jonas Allerbeck¹, Anne Marie Z Tan^{2

4}, Chengye Dong⁵, Pascal Ruffieux¹, Roman Fasel¹, Oliver Gröning¹, Yu-Chuan Lin^{3

6}, Richard G Hennig², Joshua A Robinson^{3

5

7}, Bruno Schuler⁸

Affiliations

¹ nanotech@surfaces Laboratory, Empa - Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, 8600, Switzerland.
² Department of Materials Science and Engineering, University of Florida, Gainesville, FL, 32611, USA.
³ Department of Materials Science and Engineering, The Pennsylvania State University, University Park, PA, 16082, USA.
⁴ Institute of High Performance Computing (IHPC), Agency for Science, Technology and Research (A*STAR), Singapore, 138632, Republic of Singapore.
⁵ Two-Dimensional Crystal Consortium, The Pennsylvania State University, University Park, PA, 16802, USA.
⁶ Department of Materials Science and Engineering, National Yang Ming Chiao Tung University, Hsinchu City, 300, Taiwan, ROC.
⁷ Department of Chemistry and Department of Physics, The Pennsylvania State University, University Park, PA, 16802, USA.
⁸ nanotech@surfaces Laboratory, Empa - Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, 8600, Switzerland. bruno.schuler@empa.ch.

^# Contributed equally.

PMID: 38548739
DOI: 10.1038/s41467-024-47039-4

Abstract

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 (Vac_S) and substitutional rhenium dopants (Re_Mo) can be stabilized. Vac $_{S}^{- 1}$ as well as Re $_{Mo}^{0}$ and Re $_{Mo}^{- 1}$ 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.

Abstract

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