Direct single-molecule dynamic detection of chemical reactions

Science Advances
Jianxin GuanXuefeng Guo

Abstract

Single-molecule detection can reveal time trajectories and reaction pathways of individual intermediates/transition states in chemical reactions and biological processes, which is of fundamental importance to elucidate their intrinsic mechanisms. We present a reliable, label-free single-molecule approach that allows us to directly explore the dynamic process of basic chemical reactions at the single-event level by using stable graphene-molecule single-molecule junctions. These junctions are constructed by covalently connecting a single molecule with a 9-fluorenone center to nanogapped graphene electrodes. For the first time, real-time single-molecule electrical measurements unambiguously show reproducible large-amplitude two-level fluctuations that are highly dependent on solvent environments in a nucleophilic addition reaction of hydroxylamine to a carbonyl group. Both theoretical simulations and ensemble experiments prove that this observation originates from the reversible transition between the reactant and a new intermediate state within a time scale of a few microseconds. These investigations open up a new route that is able to be immediately applied to probe fast single-molecule physics or biophysics with high time resol...Continue Reading

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Citations

Sep 6, 2019·Proceedings of the National Academy of Sciences of the United States of America·Wei-Kang WangTetsuro Majima
Sep 20, 2020·Nature Communications·Marco GobbiPaolo Samorì
May 26, 2018·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Hantao SunJianhui Liao
Jun 25, 2020·Science Advances·Chao-Yu LiJian-Feng Li
Apr 19, 2019·Chemical Science·Leopoldo Mejía, Ignacio Franco
Jun 28, 2019·Science Advances·Xiaoyan HuangWenjing Hong
Apr 4, 2020·The Journal of Chemical Physics·Caiyao YangXuefeng Guo
Nov 28, 2020·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Ivana DjurišićRadomir Zikic
Jan 7, 2021·Nanoscale·Shima Ghasemi, Kasper Moth-Poulsen
Feb 2, 2021·Science Advances·Chen YangXuefeng Guo
Mar 3, 2021·Angewandte Chemie·Linan MengSheng Meng
May 6, 2021·Chemical Communications : Chem Comm·Lu ZhangTomoaki Nishino
Jun 8, 2021·The Journal of Physical Chemistry. B·David A Nicholson, David J Nesbitt
Jul 22, 2021·Nano Letters·Xinlei YaoJean-Christophe Lacroix

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Methods Mentioned

BETA
fluorescence
optical tweezers
biosensors
chemical treatments
chip
protein folding
electron beam lithography

Software Mentioned

Gaussian
DesignCAD
QUB
Atomistix
AM1

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