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Accurate description of aqueous carbonate ions: An effective polarization model verified by neutron scattering

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Accurate description of aqueous carbonate ions : An effective polarization model verified by neutron scattering. / Mason, Philip E.; Wernersson, Erik; Jungwirth, Pavel.

In: Journal of Physical Chemistry Part B, Vol. 116, No. 28, 19.07.2012, p. 8145-8153.

Research output: Contribution to journalArticleScientificpeer-review

Harvard

Mason, PE, Wernersson, E & Jungwirth, P 2012, 'Accurate description of aqueous carbonate ions: An effective polarization model verified by neutron scattering', Journal of Physical Chemistry Part B, vol. 116, no. 28, pp. 8145-8153. https://doi.org/10.1021/jp3008267

APA

Mason, P. E., Wernersson, E., & Jungwirth, P. (2012). Accurate description of aqueous carbonate ions: An effective polarization model verified by neutron scattering. Journal of Physical Chemistry Part B, 116(28), 8145-8153. https://doi.org/10.1021/jp3008267

Vancouver

Mason PE, Wernersson E, Jungwirth P. Accurate description of aqueous carbonate ions: An effective polarization model verified by neutron scattering. Journal of Physical Chemistry Part B. 2012 Jul 19;116(28):8145-8153. https://doi.org/10.1021/jp3008267

Author

Mason, Philip E. ; Wernersson, Erik ; Jungwirth, Pavel. / Accurate description of aqueous carbonate ions : An effective polarization model verified by neutron scattering. In: Journal of Physical Chemistry Part B. 2012 ; Vol. 116, No. 28. pp. 8145-8153.

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@article{2c01c685d5c1490dbefbb22ba9330c8b,
title = "Accurate description of aqueous carbonate ions: An effective polarization model verified by neutron scattering",
abstract = "The carbonate ion plays a central role in the biochemical formation of the shells of aquatic life, which is an important path for carbon dioxide sequestration. Given the vital role of carbonate in this and other contexts, it is imperative to develop accurate models for such a high charge density ion. As a divalent ion, carbonate has a strong polarizing effect on surrounding water molecules. This raises the question whether it is possible to describe accurately such systems without including polarization. It has recently been suggested the lack of electronic polarization in nonpolarizable water models can be effectively compensated by introducing an electronic dielectric continuum, which is with respect to the forces between atoms equivalent to rescaling the ionic charges. Given how widely nonpolarizable models are used to model electrolyte solutions, establishing the experimental validity of this suggestion is imperative. Here, we examine a stringent test for such models: a comparison of the difference of the neutron scattering structure factors of K 2CO3 vs KNO3 solutions and that predicted by molecular dynamics simulations for various models of the same systems. We compare standard nonpolarizable simulations in SPC/E water to analogous simulations with effective ion charges, as well as simulations in explicitly polarizable POL3 water (which, however, has only about half the experimental polarizability). It is found that the simulation with rescaled charges is in a very good agreement with the experimental data, which is significantly better than for the nonpolarizable simulation and even better than for the explicitly polarizable POL3 model.",
author = "Mason, {Philip E.} and Erik Wernersson and Pavel Jungwirth",
year = "2012",
month = "7",
day = "19",
doi = "10.1021/jp3008267",
language = "English",
volume = "116",
pages = "8145--8153",
journal = "Journal of Physical Chemistry Part B",
issn = "1520-6106",
publisher = "American Chemical Society",
number = "28",

}

RIS (suitable for import to EndNote) - Download

TY - JOUR

T1 - Accurate description of aqueous carbonate ions

T2 - An effective polarization model verified by neutron scattering

AU - Mason, Philip E.

AU - Wernersson, Erik

AU - Jungwirth, Pavel

PY - 2012/7/19

Y1 - 2012/7/19

N2 - The carbonate ion plays a central role in the biochemical formation of the shells of aquatic life, which is an important path for carbon dioxide sequestration. Given the vital role of carbonate in this and other contexts, it is imperative to develop accurate models for such a high charge density ion. As a divalent ion, carbonate has a strong polarizing effect on surrounding water molecules. This raises the question whether it is possible to describe accurately such systems without including polarization. It has recently been suggested the lack of electronic polarization in nonpolarizable water models can be effectively compensated by introducing an electronic dielectric continuum, which is with respect to the forces between atoms equivalent to rescaling the ionic charges. Given how widely nonpolarizable models are used to model electrolyte solutions, establishing the experimental validity of this suggestion is imperative. Here, we examine a stringent test for such models: a comparison of the difference of the neutron scattering structure factors of K 2CO3 vs KNO3 solutions and that predicted by molecular dynamics simulations for various models of the same systems. We compare standard nonpolarizable simulations in SPC/E water to analogous simulations with effective ion charges, as well as simulations in explicitly polarizable POL3 water (which, however, has only about half the experimental polarizability). It is found that the simulation with rescaled charges is in a very good agreement with the experimental data, which is significantly better than for the nonpolarizable simulation and even better than for the explicitly polarizable POL3 model.

AB - The carbonate ion plays a central role in the biochemical formation of the shells of aquatic life, which is an important path for carbon dioxide sequestration. Given the vital role of carbonate in this and other contexts, it is imperative to develop accurate models for such a high charge density ion. As a divalent ion, carbonate has a strong polarizing effect on surrounding water molecules. This raises the question whether it is possible to describe accurately such systems without including polarization. It has recently been suggested the lack of electronic polarization in nonpolarizable water models can be effectively compensated by introducing an electronic dielectric continuum, which is with respect to the forces between atoms equivalent to rescaling the ionic charges. Given how widely nonpolarizable models are used to model electrolyte solutions, establishing the experimental validity of this suggestion is imperative. Here, we examine a stringent test for such models: a comparison of the difference of the neutron scattering structure factors of K 2CO3 vs KNO3 solutions and that predicted by molecular dynamics simulations for various models of the same systems. We compare standard nonpolarizable simulations in SPC/E water to analogous simulations with effective ion charges, as well as simulations in explicitly polarizable POL3 water (which, however, has only about half the experimental polarizability). It is found that the simulation with rescaled charges is in a very good agreement with the experimental data, which is significantly better than for the nonpolarizable simulation and even better than for the explicitly polarizable POL3 model.

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