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

Nature Communications
Ce ZhouXuefeng Guo

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.

References

Dec 15, 1994·Physical Review. B, Condensed Matter·P E Blöchl
Oct 28, 1996·Physical Review Letters·J P PerdewM Ernzerhof
Sep 15, 2004·Proceedings of the National Academy of Sciences of the United States of America·Fernando PatolskyCharles M Lieber
Jul 30, 2005·The Journal of Organic Chemistry·Pranjal K BaruahGangadhar J Sanjayan
Sep 7, 2006·Journal of Computational Chemistry·Stefan Grimme
Dec 20, 2007·Nano Letters·Brett R GoldsmithPhilip G Collins
Jul 23, 2009·Chemical Society Reviews·Stefan Howorka, Zuzanna Siwy
Aug 27, 2009·Proceedings of the National Academy of Sciences of the United States of America·Shuan PanJianguo Hou
Nov 16, 2010·Nature Nanotechnology·Shuo HuangStuart Lindsay
Jul 2, 2011·Physical Chemistry Chemical Physics : PCCP·Alya A Arabi, Chérif F Matta
Jan 24, 2012·Science·Yongki ChoiPhilip G Collins
Dec 12, 2012·The Journal of Physical Chemistry Letters·Chunte Sam Peng, Andrei Tokmakoff
Jan 23, 2013·Physical Chemistry Chemical Physics : PCCP·José P Cerón-Carrasco, Denis Jacquemin
Mar 16, 2013·Journal of the American Chemical Society·Tomoaki NishinoPhuc T Bui
May 22, 2013·Proceedings of the National Academy of Sciences of the United States of America·Chunte Sam PengAndrei Tokmakoff
Jan 29, 2014·Journal of the American Chemical Society·Rani AriellyYoram Selzer
Apr 8, 2014·Nature Nanotechnology·Yanan ZhaoStuart Lindsay
Jun 10, 2015·ACS Nano·Janina N LadenthinTakashi Kumagai
Jul 21, 2015·Accounts of Chemical Research·Chuancheng JiaXuefeng Guo
Dec 10, 2015·Nature Communications·Juan Manuel ArtésJoshua Hihath
Mar 17, 2016·Chemical Reviews·Dong XiangXuefeng Guo
Jun 9, 2016·Nano Letters·Delphine BouillyColin Nuckolls
Jul 29, 2016·Chemical Reviews·Jacek Waluk
Sep 24, 2016·Nature Chemistry·Janina N LadenthinTakashi Kumagai
Feb 1, 2017·Science Advances·Huimin WenXuefeng Guo

❮ Previous
Next ❯

Citations

Sep 27, 2018·Nanoscale·Xunshan LiuShi-Xia Liu
Jul 3, 2019·Physical Chemistry Chemical Physics : PCCP·Tao MaJin He
Apr 4, 2020·The Journal of Chemical Physics·Caiyao YangXuefeng Guo
May 26, 2018·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·Hantao SunJianhui Liao
Jan 1, 2021·Molecules : a Journal of Synthetic Chemistry and Natural Product Chemistry·Ying ZhangHui Wang
Nov 19, 2020·Angewandte Chemie·Štěpánka Nováková LachmanováMagdaléna Hromadová
Feb 2, 2021·Science Advances·Chen YangXuefeng Guo
Mar 3, 2021·Angewandte Chemie·Linan MengSheng Meng
Jul 22, 2021·Nano Letters·Xinlei YaoJean-Christophe Lacroix
Aug 18, 2018·ACS Nano·Paweł PuczkarskiJan A Mol
Jan 18, 2022·Journal of the American Chemical Society·Yilin GuoXuefeng Guo

❮ Previous
Next ❯

Methods Mentioned

BETA
scanning
dynamic force microscopy

Software Mentioned

TranSIESTA
Vienna initio simulation
ziControl

Related Concepts

Related Feeds

Adhesion Molecules in Health and Disease

Cell adhesion molecules are a subset of cell adhesion proteins located on the cell surface involved in binding with other cells or with the extracellular matrix in the process called cell adhesion. In essence, cell adhesion molecules help cells stick to each other and to their surroundings. Cell adhesion is a crucial component in maintaining tissue structure and function. Discover the latest research on adhesion molecule and their role in health and disease here.