Temperature dependence of the lateral hydrogen bonded clusters of molecules at the free water surface

Mária Darvas, G. Horvai, P. Jedlovszky

Research output: Contribution to journalArticle

6 Citations (Scopus)

Abstract

Molecular dynamics simulation of the liquid-vapour interface of SPC/E water have been performed on the canonical (N,V,T) ensemble in twelve temperatures ranging from 300 to 500 K using systems of two different sizes in order to locate the percolation threshold of the lateral hydrogen bonding network of surface waters. This infinite network, present at ambient conditions, is found to break up at about 450 K, i.e., 200 K below the critical temperature of the model, and hence the breakup of this two dimensional hydrogen bonding network at the liquid surface well precedes that of the three dimensional hydrogen bonding network in the bulk phase. We found that surface percolation can be described as a random bond percolation, i.e., all water molecules can form up to 3 lateral hydrogen bonds with their neighbours in the surface layer, and the formation or breaking of any of these possible hydrogen bonds is independent of that of all the other ones.

Original languageEnglish
Pages (from-to)33-38
Number of pages6
JournalJournal of Molecular Liquids
Volume176
DOIs
Publication statusPublished - Dec 2012

Fingerprint

surface water
Hydrogen
Hydrogen bonds
temperature dependence
Molecules
Water
hydrogen
molecules
hydrogen bonds
Temperature
liquid-vapor interfaces
liquid surfaces
water
Liquids
surface layers
critical temperature
Surface waters
Molecular dynamics
molecular dynamics
Vapors

Keywords

  • ITIM analysis
  • Surface percolation
  • Water liquid-vapour interface

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry
  • Spectroscopy
  • Condensed Matter Physics
  • Atomic and Molecular Physics, and Optics
  • Electronic, Optical and Magnetic Materials
  • Materials Chemistry

Cite this

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abstract = "Molecular dynamics simulation of the liquid-vapour interface of SPC/E water have been performed on the canonical (N,V,T) ensemble in twelve temperatures ranging from 300 to 500 K using systems of two different sizes in order to locate the percolation threshold of the lateral hydrogen bonding network of surface waters. This infinite network, present at ambient conditions, is found to break up at about 450 K, i.e., 200 K below the critical temperature of the model, and hence the breakup of this two dimensional hydrogen bonding network at the liquid surface well precedes that of the three dimensional hydrogen bonding network in the bulk phase. We found that surface percolation can be described as a random bond percolation, i.e., all water molecules can form up to 3 lateral hydrogen bonds with their neighbours in the surface layer, and the formation or breaking of any of these possible hydrogen bonds is independent of that of all the other ones.",
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T1 - Temperature dependence of the lateral hydrogen bonded clusters of molecules at the free water surface

AU - Darvas, Mária

AU - Horvai, G.

AU - Jedlovszky, P.

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N2 - Molecular dynamics simulation of the liquid-vapour interface of SPC/E water have been performed on the canonical (N,V,T) ensemble in twelve temperatures ranging from 300 to 500 K using systems of two different sizes in order to locate the percolation threshold of the lateral hydrogen bonding network of surface waters. This infinite network, present at ambient conditions, is found to break up at about 450 K, i.e., 200 K below the critical temperature of the model, and hence the breakup of this two dimensional hydrogen bonding network at the liquid surface well precedes that of the three dimensional hydrogen bonding network in the bulk phase. We found that surface percolation can be described as a random bond percolation, i.e., all water molecules can form up to 3 lateral hydrogen bonds with their neighbours in the surface layer, and the formation or breaking of any of these possible hydrogen bonds is independent of that of all the other ones.

AB - Molecular dynamics simulation of the liquid-vapour interface of SPC/E water have been performed on the canonical (N,V,T) ensemble in twelve temperatures ranging from 300 to 500 K using systems of two different sizes in order to locate the percolation threshold of the lateral hydrogen bonding network of surface waters. This infinite network, present at ambient conditions, is found to break up at about 450 K, i.e., 200 K below the critical temperature of the model, and hence the breakup of this two dimensional hydrogen bonding network at the liquid surface well precedes that of the three dimensional hydrogen bonding network in the bulk phase. We found that surface percolation can be described as a random bond percolation, i.e., all water molecules can form up to 3 lateral hydrogen bonds with their neighbours in the surface layer, and the formation or breaking of any of these possible hydrogen bonds is independent of that of all the other ones.

KW - ITIM analysis

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