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

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^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

4 Scopus citations

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_Mo⁰ 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.

Original language	English
Article number	2738
Journal	Nature Communications
Volume	15
Issue number	1
DOIs	https://doi.org/10.1038/s41467-024-47039-4
State	Published - Dec 2024

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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), Article 2738. https://doi.org/10.1038/s41467-024-47039-4

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title = "Charge state-dependent symmetry breaking of atomic defects in transition metal dichalcogenides",

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. 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.",

author = "Feifei Xiang and Lysander Huberich and Vargas, {Preston A.} and Riccardo Torsi and Jonas Allerbeck and Tan, {Anne Marie Z.} and Chengye Dong and Pascal Ruffieux and Roman Fasel and Oliver Gr{\"o}ning and Lin, {Yu Chuan} and Hennig, {Richard G.} and Robinson, {Joshua A.} and Bruno Schuler",

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doi = "10.1038/s41467-024-47039-4",

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AU - Huberich, Lysander

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AU - Torsi, Riccardo

AU - Allerbeck, Jonas

AU - Tan, Anne Marie Z.

AU - Dong, Chengye

AU - Ruffieux, Pascal

AU - Fasel, Roman

AU - Gröning, Oliver

AU - Lin, Yu Chuan

AU - Hennig, Richard G.

AU - Robinson, Joshua A.

AU - Schuler, Bruno

PY - 2024/12

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N2 - 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.

AB - 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.

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

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