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Toward accurate solvation dynamics of lanthanides and actinides in water using polarizable force fields: from gas-phase energetics to hydration free energies

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Abstract

In this contribution, we focused on the use of polarizable force fields to model the structural, energetic, and thermodynamical properties of lanthanides and actinides in water. In a first part, we chose the particular case of the Th(IV) cation to demonstrate the capabilities of the AMOEBA polarizable force field to reproduce both reference ab initio gas-phase energetics and experimental data including coordination numbers and radial distribution functions. Using such model, we predicted the first polarizable force field estimate of Th(IV) solvation free energy, which accounts for −1,638 kcal/mol. In addition, we proposed in a second part of this work a full extension of the SIBFA (Sum of Interaction Between Fragments Ab initio computed) polarizable potential to lanthanides (La(III) and Lu(III)) and to actinides (Th(IV)) in water. We demonstrate its capabilities to reproduce all ab initio contributions as extracted from energy decomposition analysis computations, including many-body charge transfer and discussed its applicability to extended molecular dynamics and its parametrization on high-level post-Hartree–Fock data.

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Acknowledgments

Two of the authors, C. G. and J.-P. D., thank the direction of simulation and experimental tools of the CEA nuclear energy division CEA/DEN/RBPCH for financial support. This work was granted access to the HPC resources of [CCRT/CINES/IDRIS] under the allocation x2011086146 made by GENCI (Grand Equipement National de Calcul Intensif).

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Authors and Affiliations

  1. Laboratoire de Chimie de Coordination des Eléments-f, CEA, CNRS UMR 3299, CEA Saclay, 91191, Gif-sur Yvette Cedex, France

    Aude Marjolin, Christophe Gourlaouen & Jean-Pierre Dognon

  2. Laboratoire de Chimie Théorique, UMPC, CNRS UMR 7616, CC 137 4 Place Jussieu, 75252, Paris Cedex 05, France

    Aude Marjolin & Jean-Philip Piquemal

  3. Laboratoire des Mécanismes Réactionnels, Département de Chimie, Ecole Polytechnique, CNRS, 91128, Palaiseau Cedex, France

    Carine Clavaguéra

  4. Department of Biomedical Engineering, University of Texas at Austin, Austin, TX, 78712-1062, USA

    Pengyu Y. Ren & Johnny C. Wu

  5. Laboratoire de Chimie et Biochimie Pharmacochimiques et Toxicologiques, UMR 8601 CNRS, UFR Biomédicale, Université Paris Descartes, 45 rue des Saints-Pères, 75270, Paris Cedex 06, France

    Nohad Gresh

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  1. Aude Marjolin
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Correspondence to Carine Clavaguéra, Jean-Pierre Dognon or Jean-Philip Piquemal.

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Published as part of the special collection of articles: From quantum mechanics to force fields: new methodologies for the classical simulation of complex systems.

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Marjolin, A., Gourlaouen, C., Clavaguéra, C. et al. Toward accurate solvation dynamics of lanthanides and actinides in water using polarizable force fields: from gas-phase energetics to hydration free energies. Theor Chem Acc 131, 1198 (2012). https://doi.org/10.1007/s00214-012-1198-7

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