Prindle Claudia R, Shi Wanzhuo, Li Liang, Dahl Jensen Jesper, Laursen Bo W, Steigerwald Michael L, Nuckolls Colin, Venkataraman Latha
Department of Chemistry, Columbia University, New York, New York 10027, United States.
Nano-Science Center and Department of Chemistry, University of Copenhagen, Universitetsparken 5, 2100 Copenhagen, Denmark.
J Am Chem Soc. 2024 Feb 14;146(6):3646-3650. doi: 10.1021/jacs.3c14226. Epub 2024 Jan 31.
The successful incorporation of molecules as active circuit elements relies on the ability to tune their electronic properties through chemical design. A synthetic strategy that has been used to manipulate and gate circuit conductance involves attaching a pendant substituent along the molecular conduction pathway. However, such a chemical gate has not yet been shown to significantly modify conductance. Here, we report a novel series of triarylmethylium and triangulenium carbocations gated by different substituents coupled to the delocalized conducting orbitals on the molecular backbone through a Fano resonance. By changing the pendant substituents to modulate the position of the Fano resonance and its coupling to the conducting orbitals, we can regulate the junction conductance by a remarkable factor of 450. This work thus provides a new design principle to enable effective chemical gating of single-molecule devices toward effective molecular transistors.
将分子成功整合为有源电路元件依赖于通过化学设计来调节其电子性质的能力。一种用于操纵和控制电路电导的合成策略涉及沿着分子传导路径连接一个侧链取代基。然而，这种化学门控尚未被证明能显著改变电导。在此，我们报告了一系列新型的由不同取代基门控的三芳基甲基和三角烯鎓碳正离子，它们通过法诺共振与分子主链上的离域导电轨道相连。通过改变侧链取代基来调节法诺共振的位置及其与导电轨道的耦合，我们能够将结电导调节高达450倍。因此，这项工作提供了一种新的设计原则，以实现对单分子器件进行有效的化学门控，从而制备出有效的分子晶体管。
