Enhanced Superconductivity in Few-Layer TaS2 due to Healing by Oxygenation
- Jonas Bekaert*Jonas Bekaert*Email: [email protected]Department of Physics, University of Antwerp, Groenenborgerlaan 171, B-2020 Antwerp, BelgiumMore by Jonas Bekaert
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- Ekaterina KhestanovaEkaterina KhestanovaNational Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLDepartment of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Ekaterina Khestanova
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- David G. HopkinsonDavid G. HopkinsonNational Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLDepartment of Materials, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by David G. Hopkinson
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- John BirkbeckJohn BirkbeckNational Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLDepartment of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by John Birkbeck
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- Nick ClarkNick ClarkNational Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLDepartment of Materials, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Nick Clark
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- Mengjian ZhuMengjian ZhuDepartment of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Mengjian Zhu
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- Denis A. BandurinDenis A. BandurinDepartment of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Denis A. Bandurin
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- Roman GorbachevRoman GorbachevNational Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLDepartment of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Roman Gorbachev
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- Simon FaircloughSimon FaircloughDepartment of Materials, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Simon Fairclough
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- Yichao ZouYichao ZouDepartment of Materials, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Yichao Zou
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- Matthew HamerMatthew HamerNational Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Matthew Hamer
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- Daniel J. TerryDaniel J. TerryNational Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Daniel J. Terry
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- Jonathan J. P. PetersJonathan J. P. PetersSchool of Physics, University of Warwick, Coventry, United Kingdom CV4 7ALMore by Jonathan J. P. Peters
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- Ana M. SanchezAna M. SanchezSchool of Physics, University of Warwick, Coventry, United Kingdom CV4 7ALMore by Ana M. Sanchez
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- Bart PartoensBart PartoensDepartment of Physics, University of Antwerp, Groenenborgerlaan 171, B-2020 Antwerp, BelgiumMore by Bart Partoens
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- Sarah J. Haigh*Sarah J. Haigh*Email: [email protected]National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLDepartment of Materials, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Sarah J. Haigh
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- Milorad V. Milošević*Milorad V. Milošević*Email: [email protected]Department of Physics, University of Antwerp, Groenenborgerlaan 171, B-2020 Antwerp, BelgiumMore by Milorad V. Milošević
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- Irina V. Grigorieva*Irina V. Grigorieva*Email: [email protected]National Graphene Institute, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLDepartment of Physics and Astronomy, University of Manchester, Oxford Road, Manchester, United Kingdom M13 9PLMore by Irina V. Grigorieva
Abstract

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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