Toward accurate solvation dynamics of lanthanides and actinides in water using polarizable force fields

From gas-phase energetics to hydration free energies

Aude Marjolin, Christophe Gourlaouen, Carine Clavaguéra, Pengyu Y. Ren, Johnny C. Wu, Nohad Gresh, Jean Pierre Dognon, Jean Philip Piquemal

Research output: Contribution to journalArticle

35 Citations (Scopus)

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.

Original languageEnglish
Pages (from-to)1-14
Number of pages14
JournalTheoretical Chemistry Accounts
Volume131
Issue number4
DOIs
Publication statusPublished - May 3 2012
Externally publishedYes

Fingerprint

Actinoid Series Elements
Lanthanoid Series Elements
Solvation
Hydration
field theory (physics)
Free energy
solvation
hydration
Gases
free energy
vapor phases
Water
water
Distribution functions
Molecular dynamics
Cations
Charge transfer
Decomposition
coordination number
radial distribution

Keywords

  • Actinides
  • Charge transfer
  • Energy decomposition analysis
  • Hydration free energy
  • Lanthanides
  • Polarizable force field

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Toward accurate solvation dynamics of lanthanides and actinides in water using polarizable force fields : From gas-phase energetics to hydration free energies. / Marjolin, Aude; Gourlaouen, Christophe; Clavaguéra, Carine; Ren, Pengyu Y.; Wu, Johnny C.; Gresh, Nohad; Dognon, Jean Pierre; Piquemal, Jean Philip.

In: Theoretical Chemistry Accounts, Vol. 131, No. 4, 03.05.2012, p. 1-14.

Research output: Contribution to journalArticle

Marjolin, Aude ; Gourlaouen, Christophe ; Clavaguéra, Carine ; Ren, Pengyu Y. ; Wu, Johnny C. ; Gresh, Nohad ; Dognon, Jean Pierre ; Piquemal, Jean Philip. / Toward accurate solvation dynamics of lanthanides and actinides in water using polarizable force fields : From gas-phase energetics to hydration free energies. In: Theoretical Chemistry Accounts. 2012 ; Vol. 131, No. 4. pp. 1-14.
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