Large Spin-Orbit Splitting of Deep In-Gap Defect States of Engineered Sulfur Vacancies in Monolayer WS2

Bruno Schuler; Diana Y. Qiu; Sivan Refaely-Abramson; Christoph Kastl; Christopher T. Chen; Sara Barja; Roland J. Koch; D. Frank Ogletree; Shaul Aloni; Adam M. Schwartzberg; Jeffrey B. Neaton; Steven G. Louie; Alexander Weber-Bargioni

doi:10.1103/PhysRevLett.123.076801

Large Spin-Orbit Splitting of Deep In-Gap Defect States of Engineered Sulfur Vacancies in Monolayer WS2

Bruno Schuler, Diana Y. Qiu, Sivan Refaely-Abramson, Christoph Kastl, Christopher T. Chen, Sara Barja, Roland J. Koch, D. Frank Ogletree, Shaul Aloni, Adam M. Schwartzberg, Jeffrey B. Neaton, Steven G. Louie, Alexander Weber-Bargioni

Department of Molecular Chemistry and Materials Science Perlman

Weizmann Institute of Science

Research output: Contribution to journal › Article › peer-review

Abstract

Structural defects in 2D materials offer an effective way to engineer new material functionalities beyond conventional doping. We report on the direct experimental correlation of the atomic and electronic structure of a sulfur vacancy in monolayer WS2 by a combination of CO-tip noncontact atomic force microscopy and scanning tunneling microscopy. Sulfur vacancies, which are absent in as-grown samples, were deliberately created by annealing in vacuum. Two energetically narrow unoccupied defect states followed by vibronic sidebands provide a unique fingerprint of this defect. Direct imaging of the defect orbitals, together with ab initio GW calculations, reveal that the large splitting of 252 +/- 4 meV between these defect states is induced by spin-orbit coupling.

Original language	English
Article number	076801
Number of pages	7
Journal	Physical review letters
Volume	123
Issue number	7
DOIs	https://doi.org/10.1103/PhysRevLett.123.076801
State	Published - 16 Aug 2019

All Science Journal Classification (ASJC) codes

General Physics and Astronomy

Access to Document

10.1103/PhysRevLett.123.076801

http://arxiv.org/abs/1810.02896License: Other
http://hdl.handle.net/10261/203887License: Unspecified

Cite this

Schuler, B., Qiu, D. Y., Refaely-Abramson, S., Kastl, C., Chen, C. T., Barja, S., Koch, R. J., Ogletree, D. F., Aloni, S., Schwartzberg, A. M., Neaton, J. B., Louie, S. G., & Weber-Bargioni, A. (2019). Large Spin-Orbit Splitting of Deep In-Gap Defect States of Engineered Sulfur Vacancies in Monolayer WS2. Physical review letters, 123(7), Article 076801. https://doi.org/10.1103/PhysRevLett.123.076801

@article{99c701e4abc94829aed80a47be65ca8a,

title = "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. We report on the direct experimental correlation of the atomic and electronic structure of a sulfur vacancy in monolayer WS2 by a combination of CO-tip noncontact atomic force microscopy and scanning tunneling microscopy. Sulfur vacancies, which are absent in as-grown samples, were deliberately created by annealing in vacuum. Two energetically narrow unoccupied defect states followed by vibronic sidebands provide a unique fingerprint of this defect. Direct imaging of the defect orbitals, together with ab initio GW calculations, reveal that the large splitting of 252 +/- 4 meV between these defect states is induced by spin-orbit coupling.",

author = "Bruno Schuler and Qiu, {Diana Y.} and Sivan Refaely-Abramson and Christoph Kastl and Chen, {Christopher T.} and Sara Barja and Koch, {Roland J.} and Ogletree, {D. Frank} and Shaul Aloni and Schwartzberg, {Adam M.} and Neaton, {Jeffrey B.} and Louie, {Steven G.} and Alexander Weber-Bargioni",

note = "We thank Andreas Schmid, Katherine Cochrane, and Nicholas Borys for constructive discussions. B. S. appreciates the support from the Swiss National Science Foundation under Project No. P2SKP2_171770. Theoretical work was supported by the Center for Computational Study of Excited State Phenomena in Energy Materials, which is funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-05CH11231, as part of the Computational Materials Sciences Program. The materials synthesis and STM/AFM characterization was performed at the Molecular Foundry that is supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under the same contract number. A.W.-B. and B.S. acknowledges DOE Early Career funds to perform the work. S. R.-A. acknowledges the support of Rothschild and Fulbright fellowships. S. B. acknowledges the support of the European Union under Grant No. FP7-PEOPLE-2012-IOF-327581 and of Spanish MINECO (Grant No. MAT2017-88377-C2-1-R). This research used resources of the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.",

year = "2019",

month = aug,

day = "16",

doi = "10.1103/PhysRevLett.123.076801",

language = "الإنجليزيّة",

volume = "123",

number = "7",

}

Schuler, B, Qiu, DY, Refaely-Abramson, S, Kastl, C, Chen, CT, Barja, S, Koch, RJ, Ogletree, DF, Aloni, S, Schwartzberg, AM, Neaton, JB, Louie, SG & Weber-Bargioni, A 2019, 'Large Spin-Orbit Splitting of Deep In-Gap Defect States of Engineered Sulfur Vacancies in Monolayer WS2', Physical review letters, vol. 123, no. 7, 076801. https://doi.org/10.1103/PhysRevLett.123.076801

TY - JOUR

T1 - Large Spin-Orbit Splitting of Deep In-Gap Defect States of Engineered Sulfur Vacancies in Monolayer WS2

AU - Schuler, Bruno

AU - Qiu, Diana Y.

AU - Refaely-Abramson, Sivan

AU - Kastl, Christoph

AU - Chen, Christopher T.

AU - Barja, Sara

AU - Koch, Roland J.

AU - Ogletree, D. Frank

AU - Aloni, Shaul

AU - Schwartzberg, Adam M.

AU - Neaton, Jeffrey B.

AU - Louie, Steven G.

AU - Weber-Bargioni, Alexander

N1 - We thank Andreas Schmid, Katherine Cochrane, and Nicholas Borys for constructive discussions. B. S. appreciates the support from the Swiss National Science Foundation under Project No. P2SKP2_171770. Theoretical work was supported by the Center for Computational Study of Excited State Phenomena in Energy Materials, which is funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-05CH11231, as part of the Computational Materials Sciences Program. The materials synthesis and STM/AFM characterization was performed at the Molecular Foundry that is supported by the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under the same contract number. A.W.-B. and B.S. acknowledges DOE Early Career funds to perform the work. S. R.-A. acknowledges the support of Rothschild and Fulbright fellowships. S. B. acknowledges the support of the European Union under Grant No. FP7-PEOPLE-2012-IOF-327581 and of Spanish MINECO (Grant No. MAT2017-88377-C2-1-R). This research used resources of the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.

PY - 2019/8/16

Y1 - 2019/8/16

N2 - Structural defects in 2D materials offer an effective way to engineer new material functionalities beyond conventional doping. We report on the direct experimental correlation of the atomic and electronic structure of a sulfur vacancy in monolayer WS2 by a combination of CO-tip noncontact atomic force microscopy and scanning tunneling microscopy. Sulfur vacancies, which are absent in as-grown samples, were deliberately created by annealing in vacuum. Two energetically narrow unoccupied defect states followed by vibronic sidebands provide a unique fingerprint of this defect. Direct imaging of the defect orbitals, together with ab initio GW calculations, reveal that the large splitting of 252 +/- 4 meV between these defect states is induced by spin-orbit coupling.

AB - Structural defects in 2D materials offer an effective way to engineer new material functionalities beyond conventional doping. We report on the direct experimental correlation of the atomic and electronic structure of a sulfur vacancy in monolayer WS2 by a combination of CO-tip noncontact atomic force microscopy and scanning tunneling microscopy. Sulfur vacancies, which are absent in as-grown samples, were deliberately created by annealing in vacuum. Two energetically narrow unoccupied defect states followed by vibronic sidebands provide a unique fingerprint of this defect. Direct imaging of the defect orbitals, together with ab initio GW calculations, reveal that the large splitting of 252 +/- 4 meV between these defect states is induced by spin-orbit coupling.

UR - http://www.scopus.com/inward/record.url?scp=85070855918&partnerID=8YFLogxK

U2 - 10.1103/PhysRevLett.123.076801

DO - 10.1103/PhysRevLett.123.076801

M3 - مقالة

SN - 0031-9007

VL - 123

JO - Physical review letters

JF - Physical review letters

IS - 7

M1 - 076801

ER -

Large Spin-Orbit Splitting of Deep In-Gap Defect States of Engineered Sulfur Vacancies in Monolayer WS2

Abstract

All Science Journal Classification (ASJC) codes

Access to Document

Other files and links

Fingerprint

Cite this