Local cation-tuned reversible single-molecule switch in electric double layer

Ling Tong, Zhou Yu, Yi-Jing Gao, Xiao-Chong Li, Ju-Fang Zheng, Yong Shao, Ya-Hao Wang () and Xiao-Shun Zhou ()
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Ling Tong: Zhejiang Normal University
Zhou Yu: Zhejiang Normal University
Yi-Jing Gao: Zhejiang Normal University
Xiao-Chong Li: Zhejiang Normal University
Ju-Fang Zheng: Zhejiang Normal University
Yong Shao: Zhejiang Normal University
Ya-Hao Wang: Zhejiang Normal University
Xiao-Shun Zhou: Zhejiang Normal University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract The nature of molecule-electrode interface is critical for the integration of atomically precise molecules as functional components into circuits. Herein, we demonstrate that the electric field localized metal cations in outer Helmholtz plane can modulate interfacial Au-carboxyl contacts, realizing a reversible single-molecule switch. STM break junction and I-V measurements show the electrochemical gating of aliphatic and aromatic carboxylic acids have a conductance ON/OFF behavior in electrolyte solution containing metal cations (i.e., Na+, K+, Mg2+ and Ca2+), compared to almost no change in conductance without metal cations. In situ Raman spectra reveal strong molecular carboxyl-metal cation coordination at the negatively charged electrode surface, hindering the formation of molecular junctions for electron tunnelling. This work validates the critical role of localized cations in the electric double layer to regulate electron transport at the single-molecule level.

Date: 2023
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DOI: 10.1038/s41467-023-39206-w

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