Quasi one-dimensional band dispersion and surface metallization in long-range ordered polymeric wires
Abstract
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:
-
- Univ. de Lorraine/CNRS, Nancy (France)
- Institut National de la Recherche Scientifique (INRS), Varennes, QC (Canada); Institut de Recherches sur la Catalyse et l'Environnement de Lyon, Villeurbanne (France)
- Institut National de la Recherche Scientifique (INRS), Varennes, QC (Canada)
- Institut National de la Recherche Scientifique (INRS), Varennes, QC (Canada); Queensland Univ. of Technology, Queensland (Australia)
- Institut National de la Recherche Scientifique (INRS), Varennes, QC (Canada); Univ. of Electronic Science and Technology of China, Chengdu (China)
- Instituto di Struttura della Materia, Roma (Italy)
- L'Orme des Merisiers, Gif sur Yvette (France)
- Rensselaer Polytechnic Inst., Troy, NY (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Rensselaer Polytechnic Inst., Troy, NY (United States)
- McGill Univ., Montreal QC (Canada)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1237642
- Grant/Contract Number:
- AC05-00OR22725
- Resource 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
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 36 MATERIALS SCIENCE; physical sciences; material science; condensed matter
Citation Formats
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., 2016.
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. https://doi.org/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. Mon .
"Quasi one-dimensional band dispersion and surface metallization in long-range ordered polymeric wires". United States. https://doi.org/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 = {Mon Jan 04 00:00:00 EST 2016},
month = {Mon Jan 04 00:00:00 EST 2016}
}
Web of Science
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