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

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

doi:10.1038/s41467-024-47039-4

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

Journal Article · 27 March 2024 · Nature Communications

DOI: https://doi.org/10.1038/s41467-024-47039-4 · OSTI ID:2329553

; Huberich, Lysander;

; Torsi, Riccardo;

; Tan, Anne Marie Z.; Dong, Chengye;

;

; Gröning, Oliver; Lin, Yu-Chuan;

; Robinson, Joshua A.;

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 MoS ₂ 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. $$$${\mathrm{Vac}}_{{{{{{{{\rm{S}}}}}}}}}^{-1}$$$$ ${Vac}_{S}^{- 1}$ as well as $$$${{\mathrm{Re}}}_{{{{{{{{\rm{Mo}}}}}}}}}^{0}$$$$ ${Re}_{Mo}^{0}$ and $$$${\mathrm{Re}}_{{\rm{Mo}}}^{-1}$$$$ ${Re}_{Mo}^{- 1}$ 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.

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Research Organization:: Pennsylvania State Univ., University Park, PA (United States); Univ. of Texas at Dallas, Richardson, TX (United States)

Sponsoring Organization:: European Research Council (ERC); National Science Foundation (NSF); US NIST; USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: SC0010697

OSTI ID:: 2329553

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 15; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

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

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