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

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 r...

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Published in:Nature communications 2018-02, Vol.9 (1), p.885-8, Article 885
Main Authors: Grechko, Maksim, Hasegawa, Taisuke, D’Angelo, Francesco, Ito, Hironobu, Turchinovich, Dmitry, Nagata, Yuki, Bonn, Mischa
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140/125
639/638/440/527/2257
639/638/440/94
639/638/440/948
Broadband
Coupling (molecular)
Energy dissipation
Humanities and Social Sciences
Hydrogen bonds
Infrared spectroscopy
Mathematical analysis
Molecular dynamics
multidisciplinary
Science
Science (multidisciplinary)
Spectroscopy
Spectrum analysis
Vibration
Water
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description 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. Liquid water molecules are in constant vibrational motion, but probing how their local behaviour influences collective dynamics remains a challenge. Here, the authors present terahertz-infrared spectroscopy to elucidate coupling of the O-H stretch vibration to collective, delocalized intermolecular modes.
doi_str_mv 10.1038/s41467-018-03303-y
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subjects 119/118
140/125
639/638/440/527/2257
639/638/440/94
639/638/440/948
Broadband
Coupling (molecular)
Energy dissipation
Humanities and Social Sciences
Hydrogen bonds
Infrared spectroscopy
Mathematical analysis
Molecular dynamics
multidisciplinary
Science
Science (multidisciplinary)
Spectroscopy
Spectrum analysis
Vibration
Water
title Coupling between intra- and intermolecular motions in liquid water revealed by two-dimensional terahertz-infrared-visible spectroscopy
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