Modeling the hydration of mono-atomic ...
Type de document :
Compte-rendu et recension critique d'ouvrage
DOI :
Titre :
Modeling the hydration of mono-atomic anions from the gas phase to the bulk phase: the case of the halide ions F<sup>-</sup>, Cl<sup>-</sup>, and Br<sup>-</sup>.
Auteur(s) :
Trumm, Michael [Auteur]
Institut für Nukleare Entsorgung [INE]
Guerrero Martínez, Yansel Omar [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Réal, Florent [Auteur]
Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 [PhLAM]
Masella, Michel [Auteur]
Institut de Biologie et de Technologies de Saclay [IBITECS]
Vallet, Valérie [Auteur]
Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 [PhLAM]
Schimmelpfennig, Bernd [Auteur correspondant]
Institut für Nukleare Entsorgung [INE]
Institut für Nukleare Entsorgung [INE]
Guerrero Martínez, Yansel Omar [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Réal, Florent [Auteur]
Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 [PhLAM]
Masella, Michel [Auteur]
Institut de Biologie et de Technologies de Saclay [IBITECS]
Vallet, Valérie [Auteur]
Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 [PhLAM]
Schimmelpfennig, Bernd [Auteur correspondant]
Institut für Nukleare Entsorgung [INE]
Titre de la revue :
Journal of Chemical Physics
Pagination :
044509
Éditeur :
American Institute of Physics
Date de publication :
2012-01-24
ISSN :
0021-9606
Discipline(s) HAL :
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]
Résumé en anglais : [en]
In this work, we investigate the hydration of the halide ions fluoride, chloride, and bromide using classical molecular dynamics simulations at the 10 ns scale and based on a polarizable force-field approach, which treats ...
Lire la suite >In this work, we investigate the hydration of the halide ions fluoride, chloride, and bromide using classical molecular dynamics simulations at the 10 ns scale and based on a polarizable force-field approach, which treats explicitly the cooperative bond character of strong hydrogen bond networks. We have carried out a thorough analysis of the ab initio data at the MP2 or CCSD(T) level concerning anion/water clusters in gas phase to adjust the force-field parameters. In particular, we consider the anion static polarizabilities computed in gas phase using large atomic basis sets including additional diffuse functions. The information extracted from trajectories in solution shows well structured first hydration shells formed of 6.7, 7.0, and 7.6 water molecules at about 2.78 Å, 3.15 Å, and 3.36 Å for fluoride, chloride, and bromide, respectively. These results are in excellent agreement with the latest neutron- and x-ray diffraction studies. In addition, our model reproduces several other properties of halide ions in solution, such as diffusion coefficients, description of hydration processes, and exchange reactions. Moreover, it is also able to reproduce the electrostatic properties of the anions in solution (in terms of anion dipole moment) as reported by recent ab initio quantum simulations. All the results show the ability of the proposed model in predicting data, as well as the need of accounting explicitly for the cooperative character of strong hydrogen bonds to reproduce ab initio potential energy surfaces in a mean square sense and to build up a reliable force field.Lire moins >
Lire la suite >In this work, we investigate the hydration of the halide ions fluoride, chloride, and bromide using classical molecular dynamics simulations at the 10 ns scale and based on a polarizable force-field approach, which treats explicitly the cooperative bond character of strong hydrogen bond networks. We have carried out a thorough analysis of the ab initio data at the MP2 or CCSD(T) level concerning anion/water clusters in gas phase to adjust the force-field parameters. In particular, we consider the anion static polarizabilities computed in gas phase using large atomic basis sets including additional diffuse functions. The information extracted from trajectories in solution shows well structured first hydration shells formed of 6.7, 7.0, and 7.6 water molecules at about 2.78 Å, 3.15 Å, and 3.36 Å for fluoride, chloride, and bromide, respectively. These results are in excellent agreement with the latest neutron- and x-ray diffraction studies. In addition, our model reproduces several other properties of halide ions in solution, such as diffusion coefficients, description of hydration processes, and exchange reactions. Moreover, it is also able to reproduce the electrostatic properties of the anions in solution (in terms of anion dipole moment) as reported by recent ab initio quantum simulations. All the results show the ability of the proposed model in predicting data, as well as the need of accounting explicitly for the cooperative character of strong hydrogen bonds to reproduce ab initio potential energy surfaces in a mean square sense and to build up a reliable force field.Lire moins >
Langue :
Anglais
Vulgarisation :
Non
Projet Européen :
Commentaire :
11 pages
Source :