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Title: Low-order many-body interactions determine the local structure of liquid water

Abstract

Despite its apparent simplicity, water displays unique behavior across the phase diagram which is strictly related to the ability of the water molecules to form dense, yet dynamic, hydrogen-bond networks that continually fluctuate in time and space. The competition between different local hydrogen-bonding environments has been hypothesized as a possible origin of the anomalous properties of liquid water. Through a systematic application of the many-body expansion of the total energy, we demonstrate that the local structure of liquid water at room temperature is determined by a delicate balance between two-body and three-body energies, which is further modulated by higher-order many-body effects. Besides providing fundamental insights into the structure of liquid water, this analysis also emphasizes that a correct representation of two-body and three-body energies requires sub-chemical accuracy that is nowadays only achieved by many-body models rigorously derived from the many-body expansion of the total energy, which thus hold great promise for shedding light on the molecular origin of the anomalous behavior of liquid water.

Authors:
 [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [3]
+ Show Author Affiliations
  1. Department of Chemistry and Biochemistry, University of California, La Jolla, USA
  2. San Diego Supercomputer Center, University of California, La Jolla, USA
  3. Department of Chemistry and Biochemistry, University of California, La Jolla, USA, San Diego Supercomputer Center
Publication Date:
Research Org.:
Univ. of California, San Diego, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1545172
Alternate Identifier(s):
OSTI ID: 1613249
Grant/Contract Number:  
SC0019490
Resource Type:
Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Name: Chemical Science Journal Volume: 10 Journal Issue: 35; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry

Citation Formats

Riera, Marc, Lambros, Eleftherios, Nguyen, Thuong T., Götz, Andreas W., and Paesani, Francesco. Low-order many-body interactions determine the local structure of liquid water. United Kingdom: N. p., 2019. Web. doi:10.1039/C9SC03291F.
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Riera, Marc, Lambros, Eleftherios, Nguyen, Thuong T., Götz, Andreas W., & Paesani, Francesco. Low-order many-body interactions determine the local structure of liquid water. United Kingdom. https://doi.org/10.1039/C9SC03291F
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Riera, Marc, Lambros, Eleftherios, Nguyen, Thuong T., Götz, Andreas W., and Paesani, Francesco. Wed . "Low-order many-body interactions determine the local structure of liquid water". United Kingdom. https://doi.org/10.1039/C9SC03291F.
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@article{osti_1545172,
title = {Low-order many-body interactions determine the local structure of liquid water},
author = {Riera, Marc and Lambros, Eleftherios and Nguyen, Thuong T. and Götz, Andreas W. and Paesani, Francesco},
abstractNote = {Despite its apparent simplicity, water displays unique behavior across the phase diagram which is strictly related to the ability of the water molecules to form dense, yet dynamic, hydrogen-bond networks that continually fluctuate in time and space. The competition between different local hydrogen-bonding environments has been hypothesized as a possible origin of the anomalous properties of liquid water. Through a systematic application of the many-body expansion of the total energy, we demonstrate that the local structure of liquid water at room temperature is determined by a delicate balance between two-body and three-body energies, which is further modulated by higher-order many-body effects. Besides providing fundamental insights into the structure of liquid water, this analysis also emphasizes that a correct representation of two-body and three-body energies requires sub-chemical accuracy that is nowadays only achieved by many-body models rigorously derived from the many-body expansion of the total energy, which thus hold great promise for shedding light on the molecular origin of the anomalous behavior of liquid water.},
doi = {10.1039/C9SC03291F},
journal = {Chemical Science},
number = 35,
volume = 10,
place = {United Kingdom},
year = {2019},
month = {9}
}
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https://doi.org/10.1039/C9SC03291F
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