Modeling Solubilities of Additives in Polymer Microstructures : Single-Step Perturbation Method Based on a Soft-Cavity Reference State

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2008
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Özal, Tugba A.
Hess, Berk
van der Vegt, Nico F. A.
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Macromolecules. 2008, 41(13), pp. 5055-5061. ISSN 0024-9297. eISSN 1520-5835. Available under: doi: 10.1021/ma702329q
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Solubilities of additive molecules whose molecular sizes exceed the typical dimensions of free volume cavities pre-existing in amorphous polymer melts and glasses cannot readily be computed in molecular simulations. In this paper, we perform molecular dynamics simulations of a soft-cavity reference state ensemble, which contains a soft-core, fast diffusing, Lennard-Jones particle in a rigid-chain polymer matrix. By means of the Zwanzig thermodynamic perturbation formalism, the soft particle has been perturbed to various real-solute end-states. It is shown that with this approach it is possible to overcome some of the free energy sampling problems related to the insertion of large solutes and slow diffusion in the end-state. We have calculated the excess chemical potentials of propane, chloroform, and dimethyl sulfoxide in liquid bisphenol A−polycarbonate and show that a single simulation of the reference state is sufficient to obtain statistical accuracies within error bars of 0.5−0.8 kBT. The method is particularly useful for calculating solubility ratios of large molecular solutes with approximately equal excluded volume radii.

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ISO 690ÖZAL, Tugba A., Christine PETER, Berk HESS, Nico F. A. VAN DER VEGT, 2008. Modeling Solubilities of Additives in Polymer Microstructures : Single-Step Perturbation Method Based on a Soft-Cavity Reference State. In: Macromolecules. 2008, 41(13), pp. 5055-5061. ISSN 0024-9297. eISSN 1520-5835. Available under: doi: 10.1021/ma702329q
BibTex
@article{Ozal2008-07Model-40204,
  year={2008},
  doi={10.1021/ma702329q},
  title={Modeling Solubilities of Additives in Polymer Microstructures : Single-Step Perturbation Method Based on a Soft-Cavity Reference State},
  number={13},
  volume={41},
  issn={0024-9297},
  journal={Macromolecules},
  pages={5055--5061},
  author={Özal, Tugba A. and Peter, Christine and Hess, Berk and van der Vegt, Nico F. A.}
}
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