期刊
NATURE CHEMISTRY
卷 14, 期 9, 页码 1061-+出版社
NATURE PORTFOLIO
DOI: 10.1038/s41557-022-00978-1
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资金
- National Science Foundation [DMR-1807580]
- A*STAR Graduate Academy in Singapore
- National Science Foundation Graduate Research Fellowship [DGE-1644869]
- National Defense Science and Engineering Graduate Fellowship
- Beijing Institute of Technology Research Fund Program for Young Scholars
- Project of the Science Funds of Jiangxi Education Office [GJJ180629]
- Project of Jiangxi Science and Technology Normal University [2016XJZD009]
- Deutsche Forschungsgemeinschaft (German Research Foundation) [314695032]
A family of oligophenylene-bridged bis(triarylamines) with tunable and stable mono- or di-radicaloid character was studied, showing reversed conductance decay with increasing length for oxidized wires, indicating non-classical quasi-metallic behavior.
Single-molecule topological insulators are promising candidates as conducting wires over nanometre length scales. A key advantage is their ability to exhibit quasi-metallic transport, in contrast to conjugated molecular wires which typically exhibit a low conductance that decays as the wire length increases. Here, we study a family of oligophenylene-bridged bis(triarylamines) with tunable and stable mono- or di-radicaloid character. These wires can undergo one- and two-electron chemical oxidations to the corresponding mono-cation and di-cation, respectively. We show that the oxidized wires exhibit reversed conductance decay with increasing length, consistent with the expectation for Su-Schrieffer-Heeger-type one-dimensional topological insulators. The 2.6-nm-long di-cation reported here displays a conductance greater than 0.1G(0), where G(0) is the conductance quantum, a factor of 5,400 greater than the neutral form. The observed conductance-length relationship is similar between the mono-cation and di-cation series. Density functional theory calculations elucidate how the frontier orbitals and delocalization of radicals facilitate the observed non-classical quasi-metallic behaviour.
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