Large spin-orbit splitting of deep in-gap defect states of engineered sulfur vacancies in monolayer WS2

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

doi:10.1103/physrevlett.123.076801

Title: Large spin-orbit splitting of deep in-gap defect states of engineered sulfur vacancies in monolayer WS₂

Journal Article · Thu Nov 08 00:00:00 EST 2018 · arXiv.org Repository

DOI:https://doi.org/10.1103/physrevlett.123.076801· OSTI ID:1481767

Schuler, Bruno ^[1]; Qiu, Diana Y. ^[2]; Refaely-Abramson, Sivan ^[3]; Kastl, Christoph ^[1]; Chen, Christopher T. ^[1]; Barja, Sara ^[4]; Koch, Roland J. ^[5]; Ogletree, D. Frank ^[1]; Aloni, Shaul ^[1]; Schwartzberg, Adam M. ^[1]; Neaton, Jeffrey B. ^[6]; Louie, Steven G. ^[2]; Weber-Bargioni, Alexander ^[1]

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)

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.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Swiss National Science Foundation (SNSF); European Union (EU); Ministry of Economy and Business (MINECO) (Spain)

Grant/Contract Number:: AC02-05CH11231; P2SKP2_171770; FP7-PEOPLE-2012-IOF-327581; MAT2017-88377-C2-1-R

OSTI ID:: 1481767

Alternate ID(s):: OSTI ID: 1557350

Journal Information:: arXiv.org Repository, Vol. 2018; ISSN 9999-0017

Publisher:: Cornell UniversityCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 94 works

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