Device Modelling Group, School of Engineering, University of Warwick, Coventry CV4 7AL, United Kingdom.
Nano Lett. 2023 May 10;23(9):3748-3753. doi: 10.1021/acs.nanolett.2c05068. Epub 2023 Apr 18.
Quantum interference (QI) dominates the electronic properties of single molecules even at room temperature and can lead to a large change in their electrical conductance. To take advantage of this for nanoelectronic applications, a mechanism to electronically control QI in single molecules needs to be developed. In this paper, we demonstrate that controlling the quantum interference of each spin in a stable open-shell organic radical with a large π-system is possible by changing the spin state of the radical. We show that the counterintuitive constructive spin interference in a -connected radical changes to destructive interference by changing the spin state of the radical from a doublet to a singlet. This results in a significant change in the room temperature electrical conductance by several orders of magnitude, opening up new possibilities for spin interference based molecular switches for energy storage and conversion applications.
量子干涉(QI)即使在室温下也主导着单个分子的电子性质,并可能导致其电导率发生很大变化。为了将其应用于纳米电子学,需要开发一种电子控制单个分子中 QI 的机制。在本文中,我们证明了通过改变自由基的自旋状态,可以控制具有大π系统的稳定开壳有机自由基中每个自旋的量子干涉。我们表明,通过将自由基的自旋状态从双重态改变为单重态,-连接自由基中反直觉的建设性自旋干涉变为破坏性干涉。这导致室温电导率发生了几个数量级的显著变化,为基于自旋干涉的储能和转换应用的分子开关开辟了新的可能性。