A critical assessment of methods for the intrinsic analysis of liquid interfaces. 1. surface site distributions

Miguel Jorge, Pal Jedlovszky, M. Natalia D. S. Cordeiro

Research output: Contribution to journalArticle

68 Citations (Scopus)

Abstract

Substantial progress in our understanding of interfacial structure and dynamics has stemmed from the recent development of algorithms that allow for an intrinsic analysis of fluid interfaces. These work by identifying the instantaneous location of the interface, at the atomic level, for each molecular configuration and then computing properties relative to this location. Such a procedure eliminates the broadening of the interface caused by capillary waves and reveals the underlying features of the system. However, a precise definition of which molecules actually belong to the interfacial layer is difficult to achieve in practice. Furthermore, it is not known if the different intrinsic analysis methods are consistent with each other and yield similar results for the interfacial properties. In this paper, we carry out a systematic and detailed comparison of the available methods for intrinsic analysis of fluid interfaces, based on a molecular dynamics simulation of the interface between liquid water and carbon tetrachloride. We critically assess the advantages and shortcomings of each method, based on reliability, robustness, and speed of computation, and establish consistent criteria for determining which molecules belong to the surface layer. We believe this will significantly contribute to make intrinsic analysis methods widely and routinely applicable to interfacial systems.

LanguageEnglish
Pages11169-11179
Number of pages11
JournalJournal of Physical Chemistry C
Volume114
Issue number25
Early online date9 Jun 2010
DOIs
Publication statusPublished - 1 Jul 2010

Fingerprint

Liquids
liquids
Carbon tetrachloride
Molecules
Fluids
Carbon Tetrachloride
Molecular dynamics
tetrachlorides
capillary waves
fluids
carbon tetrachloride
Water
Computer simulation
molecules
surface layers
molecular dynamics
configurations
water
simulation

Keywords

  • critical assessment
  • intrinsic analysis
  • liquid interfaces
  • surface site distributions
  • interfacial structure
  • fluid interfaces

Cite this

@article{b5f0e4524c1a43a5828a6e361d4aca5c,
title = "A critical assessment of methods for the intrinsic analysis of liquid interfaces. 1. surface site distributions",
abstract = "Substantial progress in our understanding of interfacial structure and dynamics has stemmed from the recent development of algorithms that allow for an intrinsic analysis of fluid interfaces. These work by identifying the instantaneous location of the interface, at the atomic level, for each molecular configuration and then computing properties relative to this location. Such a procedure eliminates the broadening of the interface caused by capillary waves and reveals the underlying features of the system. However, a precise definition of which molecules actually belong to the interfacial layer is difficult to achieve in practice. Furthermore, it is not known if the different intrinsic analysis methods are consistent with each other and yield similar results for the interfacial properties. In this paper, we carry out a systematic and detailed comparison of the available methods for intrinsic analysis of fluid interfaces, based on a molecular dynamics simulation of the interface between liquid water and carbon tetrachloride. We critically assess the advantages and shortcomings of each method, based on reliability, robustness, and speed of computation, and establish consistent criteria for determining which molecules belong to the surface layer. We believe this will significantly contribute to make intrinsic analysis methods widely and routinely applicable to interfacial systems.",
keywords = "critical assessment , intrinsic analysis , liquid interfaces, surface site distributions, interfacial structure , fluid interfaces",
author = "Miguel Jorge and Pal Jedlovszky and Cordeiro, {M. Natalia D. S.}",
note = "This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Journal of Physical Chemistry C, copyright {\circledC} American Chemical Society after peer review. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/jp101035r",
year = "2010",
month = "7",
day = "1",
doi = "10.1021/jp101035r",
language = "English",
volume = "114",
pages = "11169--11179",
journal = "Journal of Physical Chemistry C",
issn = "1932-7447",
publisher = "American Chemical Society",
number = "25",

}

A critical assessment of methods for the intrinsic analysis of liquid interfaces. 1. surface site distributions. / Jorge, Miguel; Jedlovszky, Pal; Cordeiro, M. Natalia D. S.

In: Journal of Physical Chemistry C, Vol. 114, No. 25, 01.07.2010, p. 11169-11179.

Research output: Contribution to journalArticle

TY - JOUR

T1 - A critical assessment of methods for the intrinsic analysis of liquid interfaces. 1. surface site distributions

AU - Jorge, Miguel

AU - Jedlovszky, Pal

AU - Cordeiro, M. Natalia D. S.

N1 - This document is the unedited Author’s version of a Submitted Work that was subsequently accepted for publication in Journal of Physical Chemistry C, copyright © American Chemical Society after peer review. To access the final edited and published work see http://pubs.acs.org/doi/abs/10.1021/jp101035r

PY - 2010/7/1

Y1 - 2010/7/1

N2 - Substantial progress in our understanding of interfacial structure and dynamics has stemmed from the recent development of algorithms that allow for an intrinsic analysis of fluid interfaces. These work by identifying the instantaneous location of the interface, at the atomic level, for each molecular configuration and then computing properties relative to this location. Such a procedure eliminates the broadening of the interface caused by capillary waves and reveals the underlying features of the system. However, a precise definition of which molecules actually belong to the interfacial layer is difficult to achieve in practice. Furthermore, it is not known if the different intrinsic analysis methods are consistent with each other and yield similar results for the interfacial properties. In this paper, we carry out a systematic and detailed comparison of the available methods for intrinsic analysis of fluid interfaces, based on a molecular dynamics simulation of the interface between liquid water and carbon tetrachloride. We critically assess the advantages and shortcomings of each method, based on reliability, robustness, and speed of computation, and establish consistent criteria for determining which molecules belong to the surface layer. We believe this will significantly contribute to make intrinsic analysis methods widely and routinely applicable to interfacial systems.

AB - Substantial progress in our understanding of interfacial structure and dynamics has stemmed from the recent development of algorithms that allow for an intrinsic analysis of fluid interfaces. These work by identifying the instantaneous location of the interface, at the atomic level, for each molecular configuration and then computing properties relative to this location. Such a procedure eliminates the broadening of the interface caused by capillary waves and reveals the underlying features of the system. However, a precise definition of which molecules actually belong to the interfacial layer is difficult to achieve in practice. Furthermore, it is not known if the different intrinsic analysis methods are consistent with each other and yield similar results for the interfacial properties. In this paper, we carry out a systematic and detailed comparison of the available methods for intrinsic analysis of fluid interfaces, based on a molecular dynamics simulation of the interface between liquid water and carbon tetrachloride. We critically assess the advantages and shortcomings of each method, based on reliability, robustness, and speed of computation, and establish consistent criteria for determining which molecules belong to the surface layer. We believe this will significantly contribute to make intrinsic analysis methods widely and routinely applicable to interfacial systems.

KW - critical assessment

KW - intrinsic analysis

KW - liquid interfaces

KW - surface site distributions

KW - interfacial structure

KW - fluid interfaces

UR - http://pubs.acs.org/journal/jpccck

U2 - 10.1021/jp101035r

DO - 10.1021/jp101035r

M3 - Article

VL - 114

SP - 11169

EP - 11179

JO - Journal of Physical Chemistry C

T2 - Journal of Physical Chemistry C

JF - Journal of Physical Chemistry C

SN - 1932-7447

IS - 25

ER -