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Enhanced Superconductivity in Few-Layer TaS2 due to Healing by Oxygenation

  • Jonas Bekaert*
    Jonas Bekaert
    Department of Physics, University of Antwerp, Groenenborgerlaan 171, B-2020 Antwerp, Belgium
    *Email: [email protected]
  • Ekaterina Khestanova
    Ekaterina Khestanova
    National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    Department of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
  • David G. Hopkinson
    David G. Hopkinson
    National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    Department of Materials, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
  • John Birkbeck
    John Birkbeck
    National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    Department of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
  • Nick Clark
    Nick Clark
    National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    Department of Materials, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    More by Nick Clark
  • Mengjian Zhu
    Mengjian Zhu
    Department of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    More by Mengjian Zhu
  • Denis A. Bandurin
    Denis A. Bandurin
    Department of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
  • Roman Gorbachev
    Roman Gorbachev
    National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    Department of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
  • Simon Fairclough
    Simon Fairclough
    Department of Materials, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
  • Yichao Zou
    Yichao Zou
    Department of Materials, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    More by Yichao Zou
  • Matthew Hamer
    Matthew Hamer
    National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
  • Daniel J. Terry
    Daniel J. Terry
    National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
  • Jonathan J. P. Peters
    Jonathan J. P. Peters
    School of Physics, University of Warwick, Coventry, United Kingdom CV4 7AL
  • Ana M. Sanchez
    Ana M. Sanchez
    School of Physics, University of Warwick, Coventry, United Kingdom CV4 7AL
  • Bart Partoens
    Bart Partoens
    Department of Physics, University of Antwerp, Groenenborgerlaan 171, B-2020 Antwerp, Belgium
  • Sarah J. Haigh*
    Sarah J. Haigh
    National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    Department of Materials, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    *Email: [email protected]
  • Milorad V. Milošević*
    Milorad V. Milošević
    Department of Physics, University of Antwerp, Groenenborgerlaan 171, B-2020 Antwerp, Belgium
    *Email: [email protected]
  • , and 
  • Irina V. Grigorieva*
    Irina V. Grigorieva
    National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    Department of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PL
    *Email: [email protected]
Cite this: Nano Lett. 2020, 20, 5, 3808–3818
Publication Date (Web):April 20, 2020
https://doi.org/10.1021/acs.nanolett.0c00871
Copyright © 2020 American Chemical Society

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    Abstract

    Abstract Image

    When approaching the atomically thin limit, defects and disorder play an increasingly important role in the properties of two-dimensional (2D) materials. While defects are generally thought to negatively affect superconductivity in 2D materials, here we demonstrate the contrary in the case of oxygenation of ultrathin tantalum disulfide (TaS2). Our first-principles calculations show that incorporation of oxygen into the TaS2 crystal lattice is energetically favorable and effectively heals sulfur vacancies typically present in these crystals, thus restoring the electronic band structure and the carrier density to the intrinsic characteristics of TaS2. Strikingly, this leads to a strong enhancement of the electron–phonon coupling, by up to 80% in the highly oxygenated limit. Using transport measurements on fresh and aged (oxygenated) few-layer TaS2, we found a marked increase of the superconducting critical temperature (Tc) upon aging, in agreement with our theory, while concurrent electron microscopy and electron-energy loss spectroscopy confirmed the presence of sulfur vacancies in freshly prepared TaS2 and incorporation of oxygen into the crystal lattice with time. Our work thus reveals the mechanism by which certain atomic-scale defects can be beneficial to superconductivity and opens a new route to engineer Tc in ultrathin materials.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.0c00871.

    • Density functional (perturbation) theory calculations; first-principles defect analysis; device fabrication; STEM-EELS analysis; identification of elements and defects in ADF-STEM imaging; analysis of EELS data; and transport measurements: sample characterization and additional data (PDF)

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