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Title: The hydrogen-bond network of water supports propagating optical phonon-like modes

Abstract

The local structure of liquid water as a function of temperature is a source of intense research. This structure is intimately linked to the dynamics of water molecules, which can be measured using Raman and infrared spectroscopies. The assignment of spectral peaks depends on whether they are collective modes or single-molecule motions. Vibrational modes in liquids are usually considered to be associated to the motions of single molecules or small clusters. Using molecular dynamics simulations, here we find dispersive optical phonon-like modes in the librational and OH-stretching bands. We argue that on subpicosecond time scales these modes propagate through water’s hydrogen-bond network over distances of up to 2 nm. In the long wavelength limit these optical modes exhibit longitudinal–transverse splitting, indicating the presence of coherent long-range dipole–dipole interactions, as in ice. Lastly, our results indicate the dynamics of liquid water have more similarities to ice than previously thought.

Authors:
 [1];  [1]
+ Show Author Affiliations
  1. Stony Brook Univ., Stony Brook, NY (United States)
Publication Date:
Research Org.:
State Univ. of New York (SUNY), Albany, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1242981
Grant/Contract Number:  
SC0003871
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
70 PLASMA PHYSICS AND FUSION TECHNOLOGY; 36 MATERIALS SCIENCE; physical sciences; physical chemistry; fluids and plasma physics

Citation Formats

Elton, Daniel C., and Fernández-Serra, Marivi. The hydrogen-bond network of water supports propagating optical phonon-like modes. United States: N. p., 2016. Web. doi:10.1038/ncomms10193.
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Elton, Daniel C., & Fernández-Serra, Marivi. The hydrogen-bond network of water supports propagating optical phonon-like modes. United States. https://doi.org/10.1038/ncomms10193
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Elton, Daniel C., and Fernández-Serra, Marivi. Mon . "The hydrogen-bond network of water supports propagating optical phonon-like modes". United States. https://doi.org/10.1038/ncomms10193. https://www.osti.gov/servlets/purl/1242981.
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@article{osti_1242981,
title = {The hydrogen-bond network of water supports propagating optical phonon-like modes},
author = {Elton, Daniel C. and Fernández-Serra, Marivi},
abstractNote = {The local structure of liquid water as a function of temperature is a source of intense research. This structure is intimately linked to the dynamics of water molecules, which can be measured using Raman and infrared spectroscopies. The assignment of spectral peaks depends on whether they are collective modes or single-molecule motions. Vibrational modes in liquids are usually considered to be associated to the motions of single molecules or small clusters. Using molecular dynamics simulations, here we find dispersive optical phonon-like modes in the librational and OH-stretching bands. We argue that on subpicosecond time scales these modes propagate through water’s hydrogen-bond network over distances of up to 2 nm. In the long wavelength limit these optical modes exhibit longitudinal–transverse splitting, indicating the presence of coherent long-range dipole–dipole interactions, as in ice. Lastly, our results indicate the dynamics of liquid water have more similarities to ice than previously thought.},
doi = {10.1038/ncomms10193},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {1}
}
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