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Title: Controllable conversion of quasi-freestanding polymer chains to graphene nanoribbons

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms14815· OSTI ID:1489365
ORCiD logo [1];  [2];  [1];  [1]; ORCiD logo [3];  [4];  [3];  [1];  [4]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  2. North Carolina State Univ., Raleigh, NC (United States). Dept. of Physics
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS) and Computer Science and Mathematics Div.
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS); North Carolina State Univ., Raleigh, NC (United States). Dept. of Physics

In the bottom-up synthesis of graphene nanoribbons (GNRs) from self-assembled linear polymer intermediates, surface-assisted cyclodehydrogenations usually take place on catalytic metal surfaces. Here we demonstrate the formation of GNRs from quasi-freestanding polymers assisted by hole injections from a scanning tunnelling microscope (STM) tip. While catalytic cyclodehydrogenations typically occur in a domino-like conversion process during the thermal annealing, the hole-injection-assisted reactions happen at selective molecular sites controlled by the STM tip. The charge injections lower the cyclodehydrogenation barrier in the catalyst-free formation of graphitic lattices, and the orbital symmetry conservation rules favour hole rather than electron injections for the GNR formation. The created polymer–GNR intraribbon heterostructures have a type-I energy level alignment and strongly localized interfacial states. Lastly, this finding points to a new route towards controllable synthesis of freestanding graphitic layers, facilitating the design of on-surface reactions for GNR-based structures.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Organization:
USDOE Office of Science (SC)
Grant/Contract Number:
FG02-98ER45685
OSTI ID:
1489365
Journal Information:
Nature Communications, Vol. 8; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 55 works
Citation information provided by
Web of Science

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Cited By (17)

Atomic‐Scale Manipulation and In Situ Characterization with Scanning Tunneling Microscopy journal October 2019
Modified Engineering of Graphene Nanoribbons Prepared via On‐Surface Synthesis journal December 2019
Design of Atomically Precise Nanoscale Negative Differential Resistance Devices journal September 2018
Supramolecular Nanostructures of Structurally Defined Graphene Nanoribbons in the Aqueous Phase journal February 2018
Supramolecular Nanostructures of Structurally Defined Graphene Nanoribbons in the Aqueous Phase journal February 2018
The art of two-dimensional soft nanomaterials journal June 2019
Ab initio investigation of the cyclodehydrogenation process for polyanthrylene transformation to graphene nanoribbons journal September 2019
Step edge-mediated assembly of periodic arrays of long graphene nanoribbons on Au(111) journal January 2019
Ultrahigh conductivity of graphene nanoribbons doped with ordered nitrogen journal January 2019
Engineered electronic states in atomically precise artificial lattices and graphene nanoribbons journal January 2019
1D metallic edge states of oxygen-terminated zigzag graphene edges journal March 2019
Top-down bottom-up graphene synthesis journal October 2019
Activating impurity effect in edge nitrogen-doped chevron graphene nanoribbons journal April 2018
Fluorine-programmed nanozipping to tailored nanographenes on rutile TiO 2 surfaces journal January 2019
Design of Atomically Precise Nanoscale Negative Differential Resistance Devices text January 2018
Engineered electronic states in atomically precise artificial lattices and graphene nanoribbons text January 2019
Step edge-mediated assembly of periodic arrays of long graphene nanoribbons on Au(111) preprint January 2019

Figures / Tables (4)


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