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Title: Quasi one-dimensional band dispersion and surface metallization in long-range ordered polymeric wires

We study the electronic structure of an ordered array of poly(para-phenylene) chains produced by surface-catalyzed dehalogenative polymerization of 1,4-dibromobenzene on copper (110). The quantization of unoccupied molecular states is measured as a function of oligomer length by scanning tunnelling spectroscopy, with Fermi level crossings observed for chains longer than ten phenyl rings. Angle-resolved photoelectron spectroscopy reveals a quasi-one-dimensional valence band as well as a direct gap of 1.15 eV, as the conduction band is partially filled through adsorption on the surface. Tight-binding modelling and ab initio density functional theory calculations lead to a full description of the organic band-structure, including the k-dispersion, the gap size and electron charge transfer mechanisms, highlighting a strong substrate-molecule interaction that drives the system into a metallic behaviour. In summary, we have fully characterized the band structure of a carbon-based conducting wire. This model system may be considered as a fingerprint of -conjugation of surface organic frameworks.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [6] ;  [6] ;  [7] ;  [7] ;  [8] ;  [9] ;  [10]
  1. Univ. de Lorraine/CNRS, Nancy (France)
  2. Institut National de la Recherche Scientifique (INRS), Varennes, QC (Canada); Institut de Recherches sur la Catalyse et l'Environnement de Lyon, Villeurbanne (France)
  3. Institut National de la Recherche Scientifique (INRS), Varennes, QC (Canada)
  4. Institut National de la Recherche Scientifique (INRS), Varennes, QC (Canada); Queensland Univ. of Technology, Queensland (Australia)
  5. Institut National de la Recherche Scientifique (INRS), Varennes, QC (Canada); Univ. of Electronic Science and Technology of China, Chengdu (China)
  6. Instituto di Struttura della Materia, Roma (Italy)
  7. L'Orme des Merisiers, Gif sur Yvette (France)
  8. Rensselaer Polytechnic Inst., Troy, NY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  9. Rensselaer Polytechnic Inst., Troy, NY (United States)
  10. McGill Univ., Montreal QC (Canada)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal Issue: 26; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
physical sciences; material science; condensed matter
OSTI Identifier:
1237642

Vasseur, Guillaume, Fagot-Revurat, Yannick, Sicot, Muriel, Kierren, Bertrand, Moreau, Luc, Malterre, Daniel, Cardenas, Luis, Galeotti, Gianluca, Lipton-Duffin, Josh, Rosei, Frederico, Giovannantonio, Marco Di, Giorgio, Contini, Fèvre, Patrick Le, Bertran, François, Liang, Liangbo, Meunier, Vincent, and Perepichka, Dmitrii F. Quasi one-dimensional band dispersion and surface metallization in long-range ordered polymeric wires. United States: N. p., Web. doi:10.1038/ncomms10235.
Vasseur, Guillaume, Fagot-Revurat, Yannick, Sicot, Muriel, Kierren, Bertrand, Moreau, Luc, Malterre, Daniel, Cardenas, Luis, Galeotti, Gianluca, Lipton-Duffin, Josh, Rosei, Frederico, Giovannantonio, Marco Di, Giorgio, Contini, Fèvre, Patrick Le, Bertran, François, Liang, Liangbo, Meunier, Vincent, & Perepichka, Dmitrii F. Quasi one-dimensional band dispersion and surface metallization in long-range ordered polymeric wires. United States. doi:10.1038/ncomms10235.
Vasseur, Guillaume, Fagot-Revurat, Yannick, Sicot, Muriel, Kierren, Bertrand, Moreau, Luc, Malterre, Daniel, Cardenas, Luis, Galeotti, Gianluca, Lipton-Duffin, Josh, Rosei, Frederico, Giovannantonio, Marco Di, Giorgio, Contini, Fèvre, Patrick Le, Bertran, François, Liang, Liangbo, Meunier, Vincent, and Perepichka, Dmitrii F. 2016. "Quasi one-dimensional band dispersion and surface metallization in long-range ordered polymeric wires". United States. doi:10.1038/ncomms10235. https://www.osti.gov/servlets/purl/1237642.
@article{osti_1237642,
title = {Quasi one-dimensional band dispersion and surface metallization in long-range ordered polymeric wires},
author = {Vasseur, Guillaume and Fagot-Revurat, Yannick and Sicot, Muriel and Kierren, Bertrand and Moreau, Luc and Malterre, Daniel and Cardenas, Luis and Galeotti, Gianluca and Lipton-Duffin, Josh and Rosei, Frederico and Giovannantonio, Marco Di and Giorgio, Contini and Fèvre, Patrick Le and Bertran, François and Liang, Liangbo and Meunier, Vincent and Perepichka, Dmitrii F.},
abstractNote = {We study the electronic structure of an ordered array of poly(para-phenylene) chains produced by surface-catalyzed dehalogenative polymerization of 1,4-dibromobenzene on copper (110). The quantization of unoccupied molecular states is measured as a function of oligomer length by scanning tunnelling spectroscopy, with Fermi level crossings observed for chains longer than ten phenyl rings. Angle-resolved photoelectron spectroscopy reveals a quasi-one-dimensional valence band as well as a direct gap of 1.15 eV, as the conduction band is partially filled through adsorption on the surface. Tight-binding modelling and ab initio density functional theory calculations lead to a full description of the organic band-structure, including the k-dispersion, the gap size and electron charge transfer mechanisms, highlighting a strong substrate-molecule interaction that drives the system into a metallic behaviour. In summary, we have fully characterized the band structure of a carbon-based conducting wire. This model system may be considered as a fingerprint of -conjugation of surface organic frameworks.},
doi = {10.1038/ncomms10235},
journal = {Nature Communications},
number = 26,
volume = 7,
place = {United States},
year = {2016},
month = {1}
}