分子二聚体连接的形成:二硫键和电压缩时间的作用

SmartMat Pub Date : 2024-03-15 DOI:10.1002/smm2.1280
Xueyan Zhao, Yan Yan, Min Tan, Surong Zhang, Xiaona Xu, Zhibin Zhao, Maoning Wang, Xubin Zhang, Adila Adijiang, Zongliang Li, E. Scheer, Dong Xiang
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引用次数: 0

摘要

由于具有出色的键合强度,带有硫醇锚定基团的苯基分子被广泛用于形成稳定的单分子连接。然而,有两个关键问题仍未得到解答,这严重阻碍了高产可靠的分子功能器件的建立:(1)是否会形成分子二聚结,如果会,二聚化是由分子间二硫键还是苯基环的π-π堆积引起的;(2)在机械压缩力作用下,分子的两个锚定基团是否有可能键合到同一个电极上,而不是桥接两个相对的电极,这将大大降低分子结的产率。在这里,我们结合大分子的紫外可见/拉曼光谱和单分子的电导/闪烁噪声测量,给出了令人信服的证据,证明分子二聚体在环境条件下自然形成,主要是通过二硫键而不是π-π堆积。我们进一步提出了一种名为 "电压缩保持(ECHO)"的技术,并揭示了苯基骨架分子的两个硫醇基团在压缩力作用下会与同一电极结合,同时延长 ECHO 时间。与此相反,烷基骨架分子则没有观察到压缩时间依赖性现象。这些史无前例的观察结果的基本机制得到了阐明,从而揭示了分子连接的产率。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Molecular dimer junctions forming: Role of disulfide bonds and electrode‐compression‐time
Thanks to their excellent bond strength, phenyl‐based molecules with thiol anchoring groups are extensively employed to form stable single‐molecule junctions. However, two critical questions are still not answered which seriously hinder high‐yield establishing reliable molecular functional devices: (1) Whether molecular dimer junctions will be formed, and if this is the case, whether the dimerization is caused by intermolecular disulfide bonds or π–π stacking of phenyl rings; (2) Upon a mechanical‐compression force, is it possible that both anchoring groups of the molecule bond to the same electrode instead of bridging two opposite electrodes, which would drastically reduce the yield of the molecular junctions. Here, combining UV‐Vis/Raman spectroscopy of bulk molecules and conductance/flicker‐noise measurements of single molecules, we give compelling evidence that molecular dimers naturally form under ambient conditions, primarily via disulfide bonds rather than by π–π stacking. We further proposed a technique, named electrode‐compression‐hold‐on (ECHO), and reveal that the two thiol groups of phenyl‐backboned molecules will bond to the same electrode upon a compression force with a prolongated ECHO time. In contrast, the compression‐time‐dependent phenomenon is not observed for alkyl‐backboned molecules. The underlying mechanism for these unprecedented observations is elucidated, shedding light on the yield of molecular junctions.
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