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 and Bruno Schuler ()
Additional contact information
Feifei Xiang: Empa – Swiss Federal Laboratories for Materials Science and Technology
Lysander Huberich: Empa – Swiss Federal Laboratories for Materials Science and Technology
Preston A. Vargas: University of Florida
Riccardo Torsi: The Pennsylvania State University
Jonas Allerbeck: Empa – Swiss Federal Laboratories for Materials Science and Technology
Anne Marie Z. Tan: University of Florida
Chengye Dong: The Pennsylvania State University
Pascal Ruffieux: Empa – Swiss Federal Laboratories for Materials Science and Technology
Roman Fasel: Empa – Swiss Federal Laboratories for Materials Science and Technology
Oliver Gröning: Empa – Swiss Federal Laboratories for Materials Science and Technology
Yu-Chuan Lin: The Pennsylvania State University
Richard G. Hennig: University of Florida
Joshua A. Robinson: The Pennsylvania State University
Bruno Schuler: Empa – Swiss Federal Laboratories for Materials Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: 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 (VacS) and substitutional rhenium dopants (ReMo) can be stabilized. $${\mathrm{Vac}}_{{{{{{{{\rm{S}}}}}}}}}^{-1}$$ Vac S − 1 as well as $${{\mathrm{Re}}}_{{{{{{{{\rm{Mo}}}}}}}}}^{0}$$ Re Mo 0 and $${\mathrm{Re}}_{{\rm{Mo}}}^{-1}$$ 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.

Date: 2024
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DOI: 10.1038/s41467-024-47039-4

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