Layer-Dependent Charge-State Lifetime of Single Se Vacancies in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"><mml:mrow><mml:msub><mml:mrow><mml:mi>WSe</mml:mi></mml:mrow><mml:mrow><mml:mn>2</mml:mn></mml:mrow></mml:msub><
Defect engineering in two-dimensional semiconductors has been exploited to tune the optoelectronic properties and introduce new quantum states in the band gap. Chalcogen vacancies in transition metal dichalcogenides in particular have been found to strongly impact charge carrier concentration and mobility in 2D transistors as well as feature subgap emission and single-photon response. In this Letter, we investigate the layer-dependent charge-state lifetime of Se vacancies in WSe_{2}. In one monolayer WSe_{2}, we observe ultrafast charge transfer from the lowest unoccupied orbital of the top Se vacancy to the graphene substrate within (1±0.2) ps measured via the current saturation in scanning tunneling approach curves. For Se vacancies decoupled by transition metal dichalcogenide (TMD) multilayers, we find a subexponential increase of the charge lifetime from (62±14) ps in bilayer to a few nanoseconds in four-layer WSe_{2}, alongside a reduction of the defect state binding energy. Additionally, we attribute the continuous suppression and energy shift of the dI/dV in-gap defect state resonances at very close tip-sample distances to a current saturation effect. Our results provide a key measure of the layer-dependent charge transfer rate of chalcogen vacancies in TMDs.
Authors
- Andres Ortega‐Guerrero (ORCID: https://orcid.org/0000-0002-0065-0623)
- Bruno Schuler (ORCID: https://orcid.org/0000-0002-9641-0340)
- Laric Bobzien (ORCID: https://orcid.org/0009-0002-9792-3567)
- Jonas Allerbeck (ORCID: https://orcid.org/0000-0002-3912-3265)
- Nils Krane (ORCID: https://orcid.org/0009-0004-6970-0846)
- Zihao Wang (ORCID: https://orcid.org/0000-0003-1999-030X)
- Daniel Figueroa
- Carlo A. Pignedoli (ORCID: https://orcid.org/0000-0002-8273-6390)
- Joshua A. Robinson (ORCID: https://orcid.org/0000-0002-1513-7187)
- Chengye Dong (ORCID: https://orcid.org/0000-0001-8598-5758)
Institutions
- Pennsylvania State University (US)
- Swiss Federal Laboratories for Materials Science and Technology (CH)
Publication Details
- Journal
- Physical Review Letters
- Published
- 2025-02-20
- DOI
- https://doi.org/10.1103/physrevlett.134.076201
- Citations
- 5
- Primary Topic
- 2D Materials and Applications
- Type
- article
- Field-Weighted Citation Impact
- 2.59
Funders
- National Science Foundation
- Werner Siemens-Stiftung
- European Commission
- Schweizerischer Nationalfonds zur Förderung der Wissenschaftlichen Forschung
- Centro Svizzero di Calcolo Scientifico
- National Supercomputing Centre Singapore
- Horizon 2020 Framework Programme
- European Research Council
- National Center of Competence in Research Materials’ Revolution: Computational Design and Discovery of Novel Materials
- Division of Materials Research
- Division of Electrical, Communications and Cyber Systems