Controllable conversion of quasi-freestanding polymer chains to graphene nanoribbons

Chuanxu Ma, Zhongcan Xiao, Honghai Zhang, Liangbo Liang, Jingsong Huang, Wenchang Lu, Bobby G. Sumpter, Kunlun Hong, J. Bernholc and An-Ping Li ()
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Chuanxu Ma: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Zhongcan Xiao: North Carolina State University
Honghai Zhang: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Liangbo Liang: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Jingsong Huang: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Wenchang Lu: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Bobby G. Sumpter: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
Kunlun Hong: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
J. Bernholc: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory
An-Ping Li: Center for Nanophase Materials Sciences, Oak Ridge National Laboratory

Nature Communications, 2017, vol. 8, issue 1, 1-7

Abstract: Abstract 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.

Date: 2017
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DOI: 10.1038/ncomms14815

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