Direct observation of single-molecule hydrogen-bond dynamics with single-bond resolution

Ce Zhou, Xingxing Li, Zhongliang Gong, Chuancheng Jia, Yuanwei Lin, Chunhui Gu, Gen He, Yuwu Zhong (), Jinlong Yang () and Xuefeng Guo ()
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Ce Zhou: Peking University
Xingxing Li: University of Science and Technology of China
Zhongliang Gong: Chinese Academy of Sciences
Chuancheng Jia: Peking University
Yuanwei Lin: Peking University
Chunhui Gu: Peking University
Gen He: Peking University
Yuwu Zhong: Chinese Academy of Sciences
Jinlong Yang: University of Science and Technology of China
Xuefeng Guo: Peking University

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract The hydrogen bond represents a fundamental interaction widely existing in nature, which plays a key role in chemical, physical and biochemical processes. However, hydrogen bond dynamics at the molecular level are extremely difficult to directly investigate. Here, in this work we address direct electrical measurements of hydrogen bond dynamics at the single-molecule and single-event level on the basis of the platform of molecular nanocircuits, where a quadrupolar hydrogen bonding system is covalently incorporated into graphene point contacts to build stable supramolecule-assembled single-molecule junctions. The dynamics of individual hydrogen bonds in different solvents at different temperatures are studied in combination with density functional theory. Both experimental and theoretical results consistently show a multimodal distribution, stemming from the stochastic rearrangement of the hydrogen bond structure mainly through intermolecular proton transfer and lactam–lactim tautomerism. This work demonstrates an approach of probing hydrogen bond dynamics with single-bond resolution, making an important contribution to broad fields beyond supramolecular chemistry.

Date: 2018
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DOI: 10.1038/s41467-018-03203-1

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