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量子干涉控制堆叠类石墨烯二聚体中的电导增强。

Quantum Interference-Controlled Conductance Enhancement in Stacked Graphene-like Dimers.

机构信息

Center of Single-Molecule Sciences, Institute of Modern Optics, Frontiers Science Center for New Organic Matter, Tianjin Key Laboratory of Micro-scale Optical Information Science and Technology, College of Electronic Information and Optical Engineering, Nankai University, 38 Tongyan Road, Jinnan District, Tianjin 300350, P. R. China.

Department of Physics, Lancaster University, Lancaster LA1 4YB, UK.

出版信息

J Am Chem Soc. 2022 Aug 31;144(34):15689-15697. doi: 10.1021/jacs.2c05909. Epub 2022 Aug 5.

Abstract

Stacking interactions are of significant importance in the fields of chemistry, biology, and material optoelectronics because they determine the efficiency of charge transfer between molecules and their quantum states. Previous studies have proven that when two monomers are π-stacked in series to form a dimer, the electrical conductance of the dimer is significantly lower than that of the monomer. Here, we present a strong opposite case that when two anthanthrene monomers are π-stacked to form a dimer in a scanning tunneling microscopic break junction, the conductance increases by as much as 25 in comparison with a monomer, which originates from a room-temperature quantum interference. Remarkably, both theory and experiment consistently reveal that this effect can be reversed by changing the connectivity of external electrodes to the monomer core. These results demonstrate that synthetic control of connectivity to molecular cores can be combined with stacking interactions between their π systems to modify and optimize charge transfer between molecules, opening up a wide variety of potential applications ranging from organic optoelectronics and photovoltaics to nanoelectronics and single-molecule electronics.

摘要

堆积相互作用在化学、生物和材料光电领域具有重要意义,因为它们决定了分子之间电荷转移及其量子态的效率。先前的研究已经证明,当两个单体通过π堆积串联形成二聚体时,二聚体的电导率明显低于单体。在这里,我们呈现了一个相反的情况,当两个蒽单体在扫描隧道显微镜断键中π堆积形成二聚体时,与单体相比,电导增加了 25,这源于室温量子干涉。值得注意的是,理论和实验都一致表明,通过改变单体核心外部电极的连接性,可以反转这种效应。这些结果表明,对分子核心连接性的合成控制可以与它们的π系统之间的堆积相互作用相结合,从而改变和优化分子之间的电荷转移,为从有机光电和光伏到纳米电子和单分子电子等各种潜在应用开辟了广阔的前景。

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