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2D Vanadium Sulfides : Synthesis, Atomic Structure Engineering, and Charge Density Waves

van Efferen, Camiel ; Hall, Joshua ; Atodiresei, Nicolae ; Boix, Virginia LU ; Safeer, Affan ; Wekking, Tobias ; Vinogradov, Nikolay A. LU orcid ; Preobrajenski, Alexei B. LU ; Knudsen, Jan LU and Fischer, Jeison , et al. (2024) In ACS Nano 18(22). p.14161-14175
Abstract

Two ultimately thin vanadium-rich 2D materials based on VS2 are created via molecular beam epitaxy and investigated using scanning tunneling microscopy, X-ray photoemission spectroscopy, and density functional theory (DFT) calculations. The controlled synthesis of stoichiometric single-layer VS2 or either of the two vanadium-rich materials is achieved by varying the sample coverage and sulfur pressure during annealing. Through annealing of small stoichiometric single-layer VS2 islands without S pressure, S-vacancies spontaneously order in 1D arrays, giving rise to patterned adsorption. Via the comparison of DFT calculations with scanning tunneling microscopy data, the atomic structure of the S-depleted... (More)

Two ultimately thin vanadium-rich 2D materials based on VS2 are created via molecular beam epitaxy and investigated using scanning tunneling microscopy, X-ray photoemission spectroscopy, and density functional theory (DFT) calculations. The controlled synthesis of stoichiometric single-layer VS2 or either of the two vanadium-rich materials is achieved by varying the sample coverage and sulfur pressure during annealing. Through annealing of small stoichiometric single-layer VS2 islands without S pressure, S-vacancies spontaneously order in 1D arrays, giving rise to patterned adsorption. Via the comparison of DFT calculations with scanning tunneling microscopy data, the atomic structure of the S-depleted phase, with a stoichiometry of V4S7, is determined. By depositing larger amounts of vanadium and sulfur, which are subsequently annealed in a S-rich atmosphere, self-intercalated ultimately thin V5S8-derived layers are obtained, which host 2 × 2 V-layers between sheets of VS2. We provide atomic models for the thinnest V5S8-derived structures. Finally, we use scanning tunneling spectroscopy to investigate the charge density wave observed in the 2D V5S8-derived islands.

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Please use this url to cite or link to this publication:
@article{99ae4863-c2d3-4004-ab52-2b26fb7ba406,
  abstract     = {{<p>Two ultimately thin vanadium-rich 2D materials based on VS<sub>2</sub> are created via molecular beam epitaxy and investigated using scanning tunneling microscopy, X-ray photoemission spectroscopy, and density functional theory (DFT) calculations. The controlled synthesis of stoichiometric single-layer VS<sub>2</sub> or either of the two vanadium-rich materials is achieved by varying the sample coverage and sulfur pressure during annealing. Through annealing of small stoichiometric single-layer VS<sub>2</sub> islands without S pressure, S-vacancies spontaneously order in 1D arrays, giving rise to patterned adsorption. Via the comparison of DFT calculations with scanning tunneling microscopy data, the atomic structure of the S-depleted phase, with a stoichiometry of V<sub>4</sub>S<sub>7</sub>, is determined. By depositing larger amounts of vanadium and sulfur, which are subsequently annealed in a S-rich atmosphere, self-intercalated ultimately thin V<sub>5</sub>S<sub>8</sub>-derived layers are obtained, which host 2 × 2 V-layers between sheets of VS<sub>2</sub>. We provide atomic models for the thinnest V<sub>5</sub>S<sub>8</sub>-derived structures. Finally, we use scanning tunneling spectroscopy to investigate the charge density wave observed in the 2D V<sub>5</sub>S<sub>8</sub>-derived islands.</p>}},
  author       = {{van Efferen, Camiel and Hall, Joshua and Atodiresei, Nicolae and Boix, Virginia and Safeer, Affan and Wekking, Tobias and Vinogradov, Nikolay A. and Preobrajenski, Alexei B. and Knudsen, Jan and Fischer, Jeison and Jolie, Wouter and Michely, Thomas}},
  issn         = {{1936-0851}},
  keywords     = {{2D materials; atomic structure engineering; charge density wave; layer dependence; transition metal dichalcogenides; VS}},
  language     = {{eng}},
  number       = {{22}},
  pages        = {{14161--14175}},
  publisher    = {{The American Chemical Society (ACS)}},
  series       = {{ACS Nano}},
  title        = {{2D Vanadium Sulfides : Synthesis, Atomic Structure Engineering, and Charge Density Waves}},
  url          = {{http://dx.doi.org/10.1021/acsnano.3c05907}},
  doi          = {{10.1021/acsnano.3c05907}},
  volume       = {{18}},
  year         = {{2024}},
}