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控制单自由基分子中的自旋干涉。

Controlling Spin Interference in Single Radical Molecules.

机构信息

Device Modelling Group, School of Engineering, University of Warwick, Coventry CV4 7AL, United Kingdom.

出版信息

Nano Lett. 2023 May 10;23(9):3748-3753. doi: 10.1021/acs.nanolett.2c05068. Epub 2023 Apr 18.

Abstract

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.

摘要

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。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/464d/10176569/a08122902812/nl2c05068_0001.jpg

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