Abstract
Substantial improvements in the molecular level understanding of fluid interfaces have recently been achieved by recognizing the importance of detecting the intrinsic surface of the coexisting condensed phases in computer simulations (i.e., after the removal of corrugations caused by capillary waves) and by developing several methods for identifying the molecules that are indeed located at the boundary of the two phases. In our previous paper [J. Phys. Chem. C 2010, 114, 11169], we critically compared those methods in terms of reliability, robustness, and computation speed. Once the intrinsic surface of a given phase is detected, various profiles, such as the density profiles of the components, can be calculated relative to this intrinsic surface rather than to the macroscopically planar Gibbs dividing surface. As a continuation of our previous study, here we present a detailed and critical comparison of various methods that can be used to calculate intrinsic density profiles once the full set of truly interfacial molecules has been identified. Two of the methods, the Fourier function and the Voronoi tessellation, are already described in the literature; two other methods, the covering surface and the triangular interpolation, are newly proposed algorithms; one method, the modified grid-based intrinsic profile (GIP) method, is an improvement over an existing procedure. The different methods are again compared in terms of accuracy and computational cost. On the basis of this comparison, we propose a fast and accurate protocol to be routinely used for intrinsic surface analyses in computer simulations.
| Original language | English |
|---|---|
| Pages (from-to) | 18656-18663 |
| Number of pages | 8 |
| Journal | Journal of Physical Chemistry C |
| Volume | 114 |
| Issue number | 43 |
| Early online date | 11 Oct 2010 |
| DOIs | |
| Publication status | Published - 4 Nov 2010 |
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Keywords
- critical assessment
- intrinsic analysis
- liquid interfaces
- density profiles
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A critical assessment of methods for the intrinsic analysis of liquid interfaces: 2. density profiles. / Jorge, Miguel; Hantal, Gyoergy; Jedlovszky, Pal; Cordeiro, M. Natalia D. S.
In: Journal of Physical Chemistry C, Vol. 114, No. 43, 04.11.2010, p. 18656-18663.Research output: Contribution to journal › Article
TY - JOUR
T1 - A critical assessment of methods for the intrinsic analysis of liquid interfaces: 2. density profiles
AU - Jorge, Miguel
AU - Hantal, Gyoergy
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 The 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/jp107378s
PY - 2010/11/4
Y1 - 2010/11/4
N2 - Substantial improvements in the molecular level understanding of fluid interfaces have recently been achieved by recognizing the importance of detecting the intrinsic surface of the coexisting condensed phases in computer simulations (i.e., after the removal of corrugations caused by capillary waves) and by developing several methods for identifying the molecules that are indeed located at the boundary of the two phases. In our previous paper [J. Phys. Chem. C 2010, 114, 11169], we critically compared those methods in terms of reliability, robustness, and computation speed. Once the intrinsic surface of a given phase is detected, various profiles, such as the density profiles of the components, can be calculated relative to this intrinsic surface rather than to the macroscopically planar Gibbs dividing surface. As a continuation of our previous study, here we present a detailed and critical comparison of various methods that can be used to calculate intrinsic density profiles once the full set of truly interfacial molecules has been identified. Two of the methods, the Fourier function and the Voronoi tessellation, are already described in the literature; two other methods, the covering surface and the triangular interpolation, are newly proposed algorithms; one method, the modified grid-based intrinsic profile (GIP) method, is an improvement over an existing procedure. The different methods are again compared in terms of accuracy and computational cost. On the basis of this comparison, we propose a fast and accurate protocol to be routinely used for intrinsic surface analyses in computer simulations.
AB - Substantial improvements in the molecular level understanding of fluid interfaces have recently been achieved by recognizing the importance of detecting the intrinsic surface of the coexisting condensed phases in computer simulations (i.e., after the removal of corrugations caused by capillary waves) and by developing several methods for identifying the molecules that are indeed located at the boundary of the two phases. In our previous paper [J. Phys. Chem. C 2010, 114, 11169], we critically compared those methods in terms of reliability, robustness, and computation speed. Once the intrinsic surface of a given phase is detected, various profiles, such as the density profiles of the components, can be calculated relative to this intrinsic surface rather than to the macroscopically planar Gibbs dividing surface. As a continuation of our previous study, here we present a detailed and critical comparison of various methods that can be used to calculate intrinsic density profiles once the full set of truly interfacial molecules has been identified. Two of the methods, the Fourier function and the Voronoi tessellation, are already described in the literature; two other methods, the covering surface and the triangular interpolation, are newly proposed algorithms; one method, the modified grid-based intrinsic profile (GIP) method, is an improvement over an existing procedure. The different methods are again compared in terms of accuracy and computational cost. On the basis of this comparison, we propose a fast and accurate protocol to be routinely used for intrinsic surface analyses in computer simulations.
KW - critical assessment
KW - intrinsic analysis
KW - liquid interfaces
KW - density profiles
UR - http://pubs.acs.org/journal/jpccck
U2 - 10.1021/jp107378s
DO - 10.1021/jp107378s
M3 - Article
VL - 114
SP - 18656
EP - 18663
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
SN - 1932-7447
IS - 43
ER -