Large spin-orbit splitting of deep in-gap defect states of engineered sulfur vacancies in monolayer WS2
Abstract
Structural defects in 2D materials offer an effective way to engineer new material functionalities beyond conventional doping in semiconductors. Specifically, deep in-gap defect states of chalcogen vacancies have been associated with intriguing phenomena in monolayer transition metal dichalcogenides (TMDs). Here, we report the direct experimental correlation of the atomic and electronic structure of a sulfur vacancy in monolayer WS2 by a combination of CO-tip non-contact atomic force microscopy (nc-AFM) and scanning tunneling microscopy (STM). Sulfur vacancies, which are absent in as-grown samples, were deliberately created by annealing in vacuum. Two energetically narrow unoccupied defect states of the vacancy provide a unique fingerprint of this defect. Direct imaging of the defect orbitals by STM and state-of-the-art GW calculations reveal that the large splitting of 252 meV between these defect states is induced by spin-orbit coupling. The controllable incorporation and potential decoration of chalcogen vacancies provide a new route to tailor the optical, catalytic and magnetic properties of TMDs.
- Authors:
-
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
- Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Physics
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of the Basque Country (UPV/EHU), Donostia (Spain). Center of Materials Physics. Dept. of Materials Physics; Basque Foundation for Science (Ikerbasque), Donostia (Spain); Donostia International Physics Center (Spain)
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Physics; Kavli Energy Nanoscience Inst. at Berkeley, CA (United States)
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); Swiss National Science Foundation (SNSF); European Union (EU); Ministry of Economy and Business (MINECO) (Spain)
- OSTI Identifier:
- 1481767
- Alternate Identifier(s):
- OSTI ID: 1557350
- Grant/Contract Number:
- AC02-05CH11231; P2SKP2_171770; FP7-PEOPLE-2012-IOF-327581; MAT2017-88377-C2-1-R
- Resource Type:
- Accepted Manuscript
- Journal Name:
- arXiv.org Repository
- Additional Journal Information:
- Journal Volume: 2018; Journal ID: ISSN 9999-0017
- Publisher:
- Cornell University
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 74 ATOMIC AND MOLECULAR PHYSICS
Citation Formats
Schuler, Bruno, Qiu, Diana Y., Refaely-Abramson, Sivan, Kastl, Christoph, Chen, Christopher T., Barja, Sara, Koch, Roland J., Ogletree, D. Frank, Aloni, Shaul, Schwartzberg, Adam M., Neaton, Jeffrey B., Louie, Steven G., and Weber-Bargioni, Alexander. Large spin-orbit splitting of deep in-gap defect states of engineered sulfur vacancies in monolayer WS2. United States: N. p., 2018.
Web. doi:10.1103/physrevlett.123.076801.
Schuler, Bruno, Qiu, Diana Y., Refaely-Abramson, Sivan, Kastl, Christoph, Chen, Christopher T., Barja, Sara, Koch, Roland J., Ogletree, D. Frank, Aloni, Shaul, Schwartzberg, Adam M., Neaton, Jeffrey B., Louie, Steven G., & Weber-Bargioni, Alexander. Large spin-orbit splitting of deep in-gap defect states of engineered sulfur vacancies in monolayer WS2. United States. doi:https://doi.org/10.1103/physrevlett.123.076801
Schuler, Bruno, Qiu, Diana Y., Refaely-Abramson, Sivan, Kastl, Christoph, Chen, Christopher T., Barja, Sara, Koch, Roland J., Ogletree, D. Frank, Aloni, Shaul, Schwartzberg, Adam M., Neaton, Jeffrey B., Louie, Steven G., and Weber-Bargioni, Alexander. Thu .
"Large spin-orbit splitting of deep in-gap defect states of engineered sulfur vacancies in monolayer WS2". United States. doi:https://doi.org/10.1103/physrevlett.123.076801. https://www.osti.gov/servlets/purl/1481767.
@article{osti_1481767,
title = {Large spin-orbit splitting of deep in-gap defect states of engineered sulfur vacancies in monolayer WS2},
author = {Schuler, Bruno and Qiu, Diana Y. and Refaely-Abramson, Sivan and Kastl, Christoph and Chen, Christopher T. and Barja, Sara and Koch, Roland J. and Ogletree, D. Frank and Aloni, Shaul and Schwartzberg, Adam M. and Neaton, Jeffrey B. and Louie, Steven G. and Weber-Bargioni, Alexander},
abstractNote = {Structural defects in 2D materials offer an effective way to engineer new material functionalities beyond conventional doping in semiconductors. Specifically, deep in-gap defect states of chalcogen vacancies have been associated with intriguing phenomena in monolayer transition metal dichalcogenides (TMDs). Here, we report the direct experimental correlation of the atomic and electronic structure of a sulfur vacancy in monolayer WS2 by a combination of CO-tip non-contact atomic force microscopy (nc-AFM) and scanning tunneling microscopy (STM). Sulfur vacancies, which are absent in as-grown samples, were deliberately created by annealing in vacuum. Two energetically narrow unoccupied defect states of the vacancy provide a unique fingerprint of this defect. Direct imaging of the defect orbitals by STM and state-of-the-art GW calculations reveal that the large splitting of 252 meV between these defect states is induced by spin-orbit coupling. The controllable incorporation and potential decoration of chalcogen vacancies provide a new route to tailor the optical, catalytic and magnetic properties of TMDs.},
doi = {10.1103/physrevlett.123.076801},
journal = {arXiv.org Repository},
number = ,
volume = 2018,
place = {United States},
year = {2018},
month = {11}
}
Web of Science
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