Journal
ADVANCED SCIENCE
Volume 9, Issue 19, Pages -Publisher
WILEY
DOI: 10.1002/advs.202200708
Keywords
curved; Diels-Alder polymerization; graphene nanoribbon; low bandgap; multi-edge structure
Categories
Funding
- EU Graphene Flagship [881603]
- H2020-MSCA-ITN (ULTIMATE) [813036]
- ERC Consolidator Grant [819698]
- Center for Advancing Electronics Dresden (cfaed) [101017821]
- DFG-SNSF Joint Switzerland-German Research Project (EnhanTopo) [429265950]
- DFG [SFB 858]
- Fonds de la Recherche Scientifique de Belgique (F.R.S.-FNRS) [2.5020.11]
- Walloon Region [1117545]
- Projekt DEAL
- [G83-28]
- [GB80-24]
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This study reports a solution synthesis method for curved graphene nanoribbons (GNRs) with hybrid edge structures. The GNRs demonstrate unique nonplanar conformation and electronic properties, including a narrow optical bandgap and high carrier mobility.
Curved graphene nanoribbons (GNRs) with hybrid edge structures have recently attracted increasing attention due to their unique band structures and electronic properties as a result of their nonplanar conformation. This work reports the solution synthesis of a long and curved multi-edged GNR (cMGNR) with unprecedented cove-armchair-gulf edge structures. The synthesis involves an efficient A(2)B(2)-type Diels-Alder polymerization between a diethynyl-substituted prefused bichrysene monomer (3b) and a dicyclopenta[e,l]pyrene-5,11-dione derivative (6) followed by FeCl3-mediated Scholl oxidative cyclodehydrogenation of the obtained polyarylenes (P1). Model compounds 1a and 1b are first synthesized to examine the suitability and efficiency of the corresponding polymers for the Scholl reaction. The successful formation of cMGNR from polymer P1 bearing prefused bichrysene units is confirmed by FTIR, Raman, and solid-state NMR analyses. The cove-edge structure of the cMGNR imparts the ribbon with a unique nonplanar conformation as revealed by density functional theory (DFT) simulation, which effectively enhances its dispersibility in solution. The cMGNR has a narrow optical bandgap of 1.61 eV, as estimated from the UV-vis absorption spectrum, which is among the family of low-bandgap solution-synthesized GNRs. Moreover, the cMGNR exhibits a carrier mobility of approximate to 2 cm(2) V-1 s(-1) inferred from contact-free terahertz spectroscopy.
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