Journal
NATURE COMMUNICATIONS
Volume 8, Issue -, Pages -Publisher
NATURE RESEARCH
DOI: 10.1038/ncomms14815
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Funding
- ONR grant [N00014-16-1-3213, N00014-16-1-3153]
- DOE [DE-FG02-98ER45685]
- Oak Ridge Associated Universities
- NSF grant at the National Center for Supercomputing Applications [OCI-1036215, NSF OCI-0725070, ACI-1238993]
- DOE at the Oak Ridge Leadership Computing Facility
- DOE at the National Energy Research Scientific Computing Center
- Eugene P. Wigner Fellowship at Oak Ridge National Laboratory
- Direct For Computer & Info Scie & Enginr
- Office of Advanced Cyberinfrastructure (OAC) [1615114] Funding Source: National Science Foundation
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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. 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.
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