Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 18, Pages 8073-8083Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c00322
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Funding
- National Natural Science Foundation of China [21788102]
- Natural Science Foundation of Guangdong Province [2019B030301003]
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Regulating charge transport within high-order structures via multiple conducting pathways provides a proof of concept for constructing multivalued logic circuits.
The construction of multivalued logic circuits by multiple quantum-interfered states at the molecular level can make full use of molecular diversity and versatility, broadening the application of molecular electronics. Understanding charge transport through different conducting pathways and how they interact with each other in molecules with a secondary structure is an indispensable foundation to achieve this goal. Herein, we elucidate the synergistic effect from through-space and through-bond conducting pathways in foldamers derived from ortho-pentaphenylene by the separate modulation on these pathways. The shrinkage of central heterocycles' sizes allows foldamers to stack with larger overlap degrees, resulting in level-crossing and thus transformation from constructive quantum interference (CQI) to destructive quantum interference (DQI) in a through-space pathway. The alteration of central heterocycles' connection sites enhances through-bond conjugation, leading to amplified contribution from a through-bond pathway. The enhanced through-bond pathway destructively interferes with the through-space pathway, exerting a suppression effect on transmission. Therefore, four quantum-interfered states of through-space and through-bond combination are generated, including through-space CQI-dominated states, through-space DQI-dominated states, through-space CQI states with through-bond suppression, and through-space DQI states with through-bond suppression. These findings enable us to regulate charge transport within high-order structures via multiple conducting pathways and provide a proof of concept to construct multivalued logic circuits.
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