Journal
ACS NANO
Volume 9, Issue 9, Pages 9228-9235Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.5b03895
Keywords
graphene; hexagonal boron nitride; bottom-up; cyclodehydrogenation; covalent network; scanning tunneling microscopy; density functional theory
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Funding
- European Research Council
- DFG Priority Program SPP 1459
- Graphene Flagship [CNECT-ICT-604391]
- European Union
- Office of Naval Research BRC Program
- Deutsche Forschungsgemeinschaft
- Swiss National Science Foundation
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We report on the bottom-up fabrication of BN-substituted heteroaromatic networks achieved by surface-assisted polymerization and subsequent cyclodehydrogenation of specifically designed BN-substituted precursor monomers based on a borazine core structural element. To get insight into the cyclodehydrogenation pathway and the influence of molecular flexibility on network quality, two closely related precursor monomers with different degrees of internal cyclodehydrogenation have been employed. Scanning tunneling microscopy shows that, for both monomers, surface-assisted cyclodehydrogenation allows for complete monomer cyclization and the formation of covalently interlinked BN-substituted polyaromatic hydrocarbon networks on the Ag(111) surface. In agreement with experimental observations, density functional theory calculations reveal a significantly lower energy barrier for the cyclodehydrogenation of the conformationally more rigid precursor monomer, which is also reflected in a higher degree of long-range order of the obtained heteroaromatic network. Our proof-of-concept study will allow for the fabrication of atomically precise substitution patterns within BNC heterostructures.
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