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

Journal Article · · arXiv.org Repository
 [1];  [2];  [3];  [1];  [1];  [4];  [5];  [1];  [1];  [1];  [6];  [2];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  2. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry; Univ. of California, Berkeley, CA (United States). Dept. of Physics
  4. 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)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source
  6. 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)
+ Show Author Affiliations

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.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Swiss National Science Foundation (SNSF); European Union (EU); Ministry of Economy and Business (MINECO) (Spain)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1481767
Journal Information:
arXiv.org Repository, Journal Name: 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 (6)

Identifying substitutional oxygen as a prolific point defect in monolayer transition metal dichalcogenides journal July 2019
Spectroscopic studies of atomic defects and bandgap renormalization in semiconducting monolayer transition metal dichalcogenides journal August 2019
Collective excitations in 2D atomic layers: Recent perspectives journal January 2020
Electron and hole transport in disordered monolayer MoS 2 : Atomic vacancy induced short-range and Coulomb disorder scattering journal September 2019
Possible realization and protection of valley-polarized quantum Hall effect in Mn / W S 2 journal January 2020
Atomistic T -matrix theory of disordered two-dimensional materials: Bound states, spectral properties, quasiparticle scattering, and transport journal January 2020

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