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Title: Orbitally Matched Edge-Doping in Graphene Nanoribbons

A series of trigonal planar N-, O-, and S-dopant atoms incorporated along the convex protrusion lining the edges of bottom-up synthesized chevron graphene nanoribbons (cGNRs) induce a characteristic shift in the energy of conduction and valence band edge states along with a significant reduction of the band gap of up to 0.3 eV per dopant atom per monomer. A combination of scanning probe spectroscopy and density functional theory calculations reveals that the direction and the magnitude of charge transfer between the dopant atoms and the cGNR backbone are dominated by inductive effects and follow the expected trend in electronegativity. The introduction of heteroatom dopants with trigonal planar geometry ensures an efficient overlap of a p-orbital lone-pair centered on the dopant atom with the extended π-system of the cGNR backbone effectively extending the conjugation length. Finally, our work demonstrates a widely tunable method for band gap engineering of graphene nanostructures for advanced electronic applications.
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [3] ;  [4] ; ORCiD logo [5]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  2. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Pohang Univ. of Science and Technology, Pohang (Korea). Dept. of Physics
  3. Pohang Univ. of Science and Technology, Pohang (Korea). Dept. of Physics
  4. Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  5. Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of California, Berkeley, CA (United States). Kavli Energy NanoSciences Inst.
Publication Date:
Grant/Contract Number:
AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 2; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Lawrence Berkeley National Laboratory-National Energy Research Scientific Computing Center
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1461127

Durr, Rebecca A., Haberer, Danny, Lee, Yea-Lee, Blackwell, Raymond, Kalayjian, Alin Miksi, Marangoni, Tomas, Ihm, Jisoon, Louie, Steven G., and Fischer, Felix R.. Orbitally Matched Edge-Doping in Graphene Nanoribbons. United States: N. p., Web. doi:10.1021/jacs.7b11886.
Durr, Rebecca A., Haberer, Danny, Lee, Yea-Lee, Blackwell, Raymond, Kalayjian, Alin Miksi, Marangoni, Tomas, Ihm, Jisoon, Louie, Steven G., & Fischer, Felix R.. Orbitally Matched Edge-Doping in Graphene Nanoribbons. United States. doi:10.1021/jacs.7b11886.
Durr, Rebecca A., Haberer, Danny, Lee, Yea-Lee, Blackwell, Raymond, Kalayjian, Alin Miksi, Marangoni, Tomas, Ihm, Jisoon, Louie, Steven G., and Fischer, Felix R.. 2017. "Orbitally Matched Edge-Doping in Graphene Nanoribbons". United States. doi:10.1021/jacs.7b11886. https://www.osti.gov/servlets/purl/1461127.
@article{osti_1461127,
title = {Orbitally Matched Edge-Doping in Graphene Nanoribbons},
author = {Durr, Rebecca A. and Haberer, Danny and Lee, Yea-Lee and Blackwell, Raymond and Kalayjian, Alin Miksi and Marangoni, Tomas and Ihm, Jisoon and Louie, Steven G. and Fischer, Felix R.},
abstractNote = {A series of trigonal planar N-, O-, and S-dopant atoms incorporated along the convex protrusion lining the edges of bottom-up synthesized chevron graphene nanoribbons (cGNRs) induce a characteristic shift in the energy of conduction and valence band edge states along with a significant reduction of the band gap of up to 0.3 eV per dopant atom per monomer. A combination of scanning probe spectroscopy and density functional theory calculations reveals that the direction and the magnitude of charge transfer between the dopant atoms and the cGNR backbone are dominated by inductive effects and follow the expected trend in electronegativity. The introduction of heteroatom dopants with trigonal planar geometry ensures an efficient overlap of a p-orbital lone-pair centered on the dopant atom with the extended π-system of the cGNR backbone effectively extending the conjugation length. Finally, our work demonstrates a widely tunable method for band gap engineering of graphene nanostructures for advanced electronic applications.},
doi = {10.1021/jacs.7b11886},
journal = {Journal of the American Chemical Society},
number = 2,
volume = 140,
place = {United States},
year = {2017},
month = {12}
}