Synchronized Photoluminescence and Electrical Mobility Enhancement in 2D WS <sub>2</sub> through Sequence-Specific Chemical Passivation
Two-dimensional (2D) semiconducting dichalcogenides hold exceptional promise for next-generation electronic and photonic devices. Despite this potential, the pervasive presence of defects in 2D dichalcogenides results in carrier mobility and photoluminescence (PL) that fall significantly short of theoretical predictions. Although defect passivation offers a potential solution, its effects have been inconsistent. This arises from the lack of chemical understanding of the surface chemistry of the 2D material. In this work, we uncover new binding chemistry using a sequence-specific chemical passivation (SSCP) protocol based on 2-furanmethanothiol (FSH) and bis(trifluoromethane) sulfonimide lithium salt (Li-TFSI), which demonstrates a synchronized 100-fold enhancement in both carrier mobility and PL in WS<sub>2</sub> monolayers. We propose an atomic-level synergistic defect passivation mechanism of both neutral and charged sulfur vacancies (SVs), supported by ultrafast transient absorption spectroscopy (TA), Hard X-ray photoelectron spectroscopy (HAXPES), and density functional theory (DFT) calculations. Our results establish a new semiconductor quality benchmark for 2D WS<sub>2</sub>, paving the way for the development of sustainable 2D semiconductor technologies.
Authors
- Deepa Thakur (ORCID: https://orcid.org/0000-0001-9736-2988)
- T. Kimura (ORCID: https://orcid.org/0000-0002-1253-2130)
- Ulrich Nguétchuissi Noumbé
- Andreas Lindblad (ORCID: https://orcid.org/0000-0002-9188-9604)
- Makoto Kohda (ORCID: https://orcid.org/0000-0002-1995-1282)
- Tomas Edvinsson (ORCID: https://orcid.org/0000-0003-2759-7356)
- Rafael B. Araujo (ORCID: https://orcid.org/0000-0002-3964-2807)
- Eito Asakura
- Akshay Rao (ORCID: https://orcid.org/0000-0003-4261-0766)
- Victor Gray (ORCID: https://orcid.org/0000-0001-6583-8654)
- M. Venkata Kamalakar (ORCID: https://orcid.org/0000-0003-2385-9267)
- Elin Berggren (ORCID: https://orcid.org/0000-0001-8693-0492)
- Henry Nameirakpam (ORCID: https://orcid.org/0009-0008-6675-8603)
- Zhaojun Li (ORCID: https://orcid.org/0000-0003-2651-1717)
Institutions
- Uppsala University (SE)
- Solid State Physics Laboratory (IN)
- Tohoku University (JP)
- University of Cambridge (GB)
- Laboratoire de physique des Solides (FR)
- Bridge University (SS)
- Angstrom Designs (United States) (US)
- Astronomy and Space (AU)
- Institute of Solid State Physics (CN)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2024-12-11
- DOI
- https://doi.org/10.1021/jacs.4c11052
- Citations
- 11
- Primary Topic
- 2D Materials and Applications
- Type
- article
- Field-Weighted Citation Impact
- 1.29
Funders
- Bertil and Britt Svenssons Stiftelse för Belysningsteknik
- Göran Gustafssons Stiftelser
- European Commission
- Svenska Forskningsrådet Formas
- Vetenskapsrådet
- Uppsala Universitet
- Stiftelsen Åforsk
- European Research Council