Xu Xiaohui, Wang Juejun, Blankevoort Nickel, Daaoub Abdalghani, Sangtarash Sara, Shi Jie, Fang Chao, Yuan Saisai, Chen Lichuan, Liu Junyang, Yang Yang, Sadeghi Hatef, Hong Wenjing
State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering & Pen-Tung Sah Institute of Micro-Nano Science and Technology, IKKEM, Xiamen University, Xiamen 361005, China.
Device Modelling Group, School of Engineering, University of Warwick, CV4 7AL Coventry, United Kingdom.
Proc Natl Acad Sci U S A. 2022 Nov 16;119(46):e2211786119. doi: 10.1073/pnas.2211786119. Epub 2022 Nov 7.
The discovery of quantum interference (QI) is widely considered as an important advance in molecular electronics since it provides unique opportunities for achieving single-molecule devices with unprecedented performance. Although some pioneering studies suggested the presence of spin qubit coherence and QI in collective systems such as thin films, it remains unclear whether the QI can be transferred step-by-step from single molecules to different length scales, which hinders the application of QI in fabricating active molecular devices. Here, we found that QI can be transferred from a single molecule to their assemblies. We synthesized and investigated the charge transport through the molecular cages using 1,3-dipyridylbenzene (DPB) as a ligand block with a destructive quantum interference (DQI) effect and 2,5-dipyridylfuran (DPF) as a control building block with a constructive quantum interference (CQI) effect using both single-molecule break junction and large area junction techniques. Combined experiments and calculations revealed that both DQI and CQI had been transferred from the ligand blocks to the molecular cages and the monolayer thin film of the cages. Our work introduced QI effects from a ligand to the molecular cage comprising 732 atoms and even their monolayers, suggesting that the quantum interference could be scaled up within the phase-coherent distance.
量子干涉(QI)的发现被广泛认为是分子电子学领域的一项重要进展,因为它为实现具有前所未有的性能的单分子器件提供了独特的机会。尽管一些开创性研究表明在诸如薄膜等集体系统中存在自旋量子比特相干性和量子干涉,但尚不清楚量子干涉是否能从单分子逐步转移到不同的长度尺度,这阻碍了量子干涉在制造有源分子器件中的应用。在此,我们发现量子干涉可以从单分子转移到它们的组装体。我们合成并研究了通过分子笼的电荷传输,使用具有破坏性量子干涉(DQI)效应的1,3 - 二吡啶基苯(DPB)作为配体块,以及具有建设性量子干涉(CQI)效应的2,5 - 二吡啶基呋喃(DPF)作为对照构建块,采用单分子断结和大面积结技术。结合实验和计算表明,DQI和CQI都已从配体块转移到分子笼以及笼的单层薄膜中。我们的工作将量子干涉效应从配体引入到包含732个原子的分子笼甚至其单层中,表明量子干涉可以在相位相干距离内进行扩展。