Understanding the Role of Parallel Pathways via In-Situ Switching of Quantum Interference in Molecular Tunneling Junctions.,Angewandte Chemie International Edition

当前位置： X-MOL 学术 › Angew. Chem. Int. Ed. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Understanding the Role of Parallel Pathways via In-Situ Switching of Quantum Interference in Molecular Tunneling Junctions.
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-05-29 , DOI: 10.1002/anie.202005047
Saurabh Soni _{1,

2} , Gang Ye _{1,

2,

3} , Jueting Zheng ₄ , Yanxi Zhang _{1,

2,

5} , Andika Asyuda ₆ , Michael Zharnikov ₆ , Wenjing Hong ₄ , Ryan C Chiechi _{1,

2}

Affiliation

This study describes the modulation of tunneling probabilities in molecular junctions by switching one of two parallel intramolecular pathways. A linearly conjugated molecular wire provides a rigid framework that allows a second, cross‐conjugated pathway to be effectively switched on and off by protonation, affecting the total conductance of the junction. This approach works because a traversing electron interacts with the entire quantum‐mechanical circuit simultaneously; Kirchhoff's rules do not apply. We confirm this concept by comparing the conductances of a series of compounds with single or parallel pathways in large‐area junctions using EGaIn contacts and single‐molecule break junctions using gold contacts. We affect switching selectively in one of two parallel pathways by converting a cross‐conjugated carbonyl carbon into a trivalent carbocation, which replaces destructive quantum interference with a symmetrical resonance, causing an increase in transmission in the bias window.

中文翻译：

通过分子隧道结中量子干扰的原位切换了解平行通路的作用。

这项研究描述了通过切换两个平行分子内路径之一来调节分子连接中的隧道概率。线性共轭分子线提供了一个刚性框架，允许通过质子化有效地打开和关闭第二条交叉共轭路径，从而影响结的总电导。这种方法之所以有效，是因为穿过的电子同时与整个量子力学电路相互作用。基尔霍夫规则不适用。我们通过比较使用 EGaIn 接触的大面积结和使用金接触的单分子断裂结中具有单一或平行路径的一系列化合物的电导来证实这一概念。我们通过将交叉共轭的羰基碳转化为三价碳阳离子，选择性地影响两个平行路径之一的切换，这用对称共振取代了破坏性的量子干扰，导致偏置窗口中的传输增加。

更新日期：2020-05-29

点击分享查看原文

点击收藏

公开下载

阅读更多本刊最新论文本刊介绍/投稿指南11