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^*

^*此作品的通信作者

研究成果: Article › 同行評審

11 引文斯高帕斯（Scopus）

摘要

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.

原文	English
文章編號	2738
期刊	Nature Communications
卷	15
發行號	1
DOIs	https://doi.org/10.1038/s41467-024-47039-4
出版狀態	Published - 12月 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), 文章 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 - Xiang, Feifei

AU - Huberich, Lysander

AU - Vargas, Preston A.

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

Y1 - 2024/12

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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