Stereoelectronic Switches of Single-Molecule Junctions through Conformation-Modulated Intramolecular Coupling Approaches

IF 4.8 2区 化学 Q2 CHEMISTRY, PHYSICAL The Journal of Physical Chemistry Letters Pub Date : 2023-10-19 DOI:10.1021/acs.jpclett.3c02577
Zhuan-Yun Cai, Zi-Wei Ma, Wen-Kai Wu, Jian-De Lin, Lin-Qi Pei, Jia-Zheng Wang, Tai-Rui Wu, Shan Jin, De-Yin Wu* and Zhong-Qun Tian, 
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Abstract

Stereoelectronic effects in single-molecule junctions have been widely utilized to achieve a molecular switch, but high-efficiency and reproducible switching remain challenging. Here, we demonstrate that there are three stable intramolecular conformations in the 9,10-diphenyl-9,10-methanoanthracen-11-one (DPMAO) systems due to steric effect. Interestingly, different electronic coupling approaches including weak coupling (through-space), decoupling, and strong coupling (through-bond) between two terminal benzene rings are accomplished in the three stable conformations, respectively. Theoretical calculations show that the molecular conductance of three stable conformations differs by more than 1 order of magnitude. Furthermore, the populations of the three stable conformations are highly dependent on the solvent effect and the external electric field. Therefore, an excellent molecular switch can be achieved using the DPMAO molecule junctions and external stimuli. Our findings reveal that modulating intramolecular electronic coupling approaches may be a useful manner to enable molecular switches with high switching ratios. This opens up a new route for building high-efficiency molecular switches in single-molecular junctions.

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通过构象调制分子内耦合方法实现单分子连接的立体电子开关。
单分子结中的立体电子效应已被广泛用于实现分子开关,但高效和可重复的开关仍然具有挑战性。在这里,我们证明了由于空间效应,在9,10-二苯基-9,10-甲蒽-11酮(DPMAO)体系中存在三种稳定的分子内构象。有趣的是,不同的电子耦合方法,包括两个末端苯环之间的弱耦合(通过空间)、去耦和强耦合(通过键),分别在三种稳定构象中实现。理论计算表明,三种稳定构象的分子电导相差超过1个数量级。此外,三种稳定构象的布居高度依赖于溶剂效应和外部电场。因此,使用DPMAO分子连接和外部刺激可以实现极好的分子开关。我们的发现表明,调节分子内电子耦合方法可能是实现高开关比的分子开关的有用方式。这为在单分子结中构建高效分子开关开辟了一条新途径。
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来源期刊
The Journal of Physical Chemistry Letters
The Journal of Physical Chemistry Letters CHEMISTRY, PHYSICAL-NANOSCIENCE & NANOTECHNOLOGY
CiteScore
9.60
自引率
7.00%
发文量
1519
审稿时长
1.6 months
期刊介绍: The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.
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