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 · 28 March 2024 · Nature Communications

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

^[1]; Huberich, Lysander ^[1];

^[2]; Torsi, Riccardo ^[3];

^[1]; Tan, Anne Marie Z. ^[4]; Dong, Chengye ^[3];

^[1];

^[1]; Gröning, Oliver ^[1]; Lin, Yu-Chuan ^[5];

^[2]; Robinson, Joshua A. ^[3];

^[1]

Swiss Federal Laboratories for Materials Science and Technology (Empa), Dübendorf (Switzerland)
Univ. of Florida, Gainesville, FL (United States)
Pennsylvania State Univ., University Park, PA (United States)
Univ. of Florida, Gainesville, FL (United States); Agency for Science, Technology and Research (A*STAR) (Singapore)
Pennsylvania State Univ., University Park, PA (United States); National Yang Ming Chiao Tung Univ., Hsinchu City (Taiwan)

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. $$Vac^{-1}_{S}$$ as well as $$Re^{0}_{Mo}$$ and $$Re^{-1}_{Mo}$$ 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:: Univ. of Texas at Dallas, Richardson, TX (United States); Pennsylvania State Univ., University Park, PA (United States)

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

Grant/Contract Number:: SC0010697; DESC0010697

OSTI ID:: 2329553

Alternate ID(s):: OSTI ID: 2472342

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

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
atomic quantum emitters
lattice coordination
symmetry

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

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