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Single spin defects in 2D transition-metal dichalcogenides are natural spin-photon interfaces for quantum applications. Here we report high-field magneto-photoluminescence spectroscopy from three emission lines (Q1, Q2 and Q*) of He-ion induced sulfur vacancies in monolayer MoS2. Analysis of the asymmetric PL lineshapes in combination with the diamagnetic shift of Q1 and Q2 yields a consistent picture of localized emitters with a wavefunction extent of 2-3nm. The distinct valley- Zeeman splitting in out-of-plane B-fields and the brightening of dark states through in-plane B-fields necessitates lifting of the spin-degeneracy at zero field. Comparing our results to ab-inito calculations unambiguously identifies the nature of Q1 and Q2 and suggests that Q* is the emission from a chemically functionalized defect. Analysis of the optical degree of circular polarization reveals that the Fermi level is a parameter that enables the tunability of the spin-defect. These results highlight that defects in 2D semiconductors may be utilized for quantum technologies.

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• Creative Commons BY Attribution 4.0 International
  

Keyword: Spin-defects, magneto-photoluminescence, sulfur vacancies

Date published: 2023-04-08

Publisher: Springer Science and Business Media LLC

Journal:

• npj 2D Materials and Applications (ISSN: 23977132) vol. 7 issue. 1 30

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Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1038/s41699-023-00392-2

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Updated at: 2025-02-23 22:48:02 +0900

Published on MDR: 2025-02-23 22:48:02 +0900