Coupling between intra- and intermolecular motions in liquid water revealed by two-dimensional terahertz-infrared-visible spectroscopy

Nature Communications
Maksim GrechkoMischa Bonn

Abstract

The interaction between intramolecular and intermolecular degrees of freedom in liquid water underlies fundamental chemical and physical phenomena such as energy dissipation and proton transfer. Yet, it has been challenging to elucidate the coupling between these different types of modes. Here, we report on the direct observation and quantification of the coupling between intermolecular and intramolecular coordinates using two-dimensional, ultra-broadband, terahertz-infrared-visible (2D TIRV) spectroscopy and molecular dynamics calculations. Our study reveals strong coupling of the O-H stretch vibration, independent of the degree of delocalization of this high-frequency mode, to low-frequency intermolecular motions over a wide frequency range from 50 to 250 cm-1, corresponding to both the intermolecular hydrogen bond bending (≈ 60 cm-1) and stretching (≈ 180 cm-1) modes. Our results provide mechanistic insights into the coupling of the O-H stretch vibration to collective, delocalized intermolecular modes.

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Citations

Aug 16, 2018·Angewandte Chemie·Maksim GrechkoMischa Bonn
Jan 16, 2020·Physical Chemistry Chemical Physics : PCCP·Tian TianSamantha Jenkins
Jun 25, 2018·The Journal of Chemical Physics·Saima AhmedPeter Hamm
Feb 3, 2019·The Journal of Chemical Physics·David Sidler, Peter Hamm
Jan 30, 2019·Proceedings of the National Academy of Sciences of the United States of America·Arian BergerAndrey Shalit
Feb 18, 2021·Physical Chemistry Chemical Physics : PCCP·Juin W Zhou, M Hassan Arbab
Mar 13, 2021·Physical Chemistry Chemical Physics : PCCP·Aritri Biswas, Bhabani S Mallik
Apr 4, 2021·The Journal of Chemical Physics·Klaus ReimannThomas Elsaesser
May 6, 2021·Physical Chemistry Chemical Physics : PCCP·Hong-Fei YeZhen Chen
Jun 23, 2021·The Journal of Physical Chemistry Letters·Federico CaporalettiSander Woutersen
Jul 10, 2021·The Journal of Chemical Physics·Laura VietzeMaksim Grechko
Nov 26, 2019·The Journal of Physical Chemistry Letters·Laetitia DalsteinBertrand Busson
Nov 24, 2020·The Journal of Physical Chemistry. B·Vasily G ArtemovHenni Ouerdane
Dec 15, 2020·The Journal of Physical Chemistry Letters·Taija L FischerMartin A Suhm
Jan 7, 2021·The Journal of Physical Chemistry. B·A ShalitP Hamm
Mar 10, 2020·Journal of Chemical Theory and Computation·Seiji Ueno, Yoshitaka Tanimura

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