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Polarizability rescaling and atom-based Thole scaling in the CHARMM Drude polarizable force field for ethers

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Abstract

Within the CHARMM polarizable force field based on the classical Drude oscillator, atomic polarizabilities are derived via fitting to ab initio calculated data on isolated gas phase molecules, with an empirical scaling factor applied to account for differences between the gas and condensed phases. In the development of polarizable models for the ethers, a polarizability scaling factor of 0.7 was previously applied [Vorobyov et al. J Comput Chem 3:1120–1133, 2007]. While the resulting force field models gave good agreement with a variety of experimental data, they systematically underestimated the liquid phase dielectric constants. Here, a new CHARMM polarizable model is developed for the ethers, employing a polarizability scaling factor of 0.85 and including atom-based Thole scale factors recently introduced into the CHARMM Drude polarizable force field [Harder et al. J Phys Chem B 112:3509-3521, 2008]. The new model offers a significant improvement in the reproduction of liquid phase dielectric constants, while maintaining the good agreement of the previous model with all other experimental and quantum mechanical data, highlighting the sensitivity of liquid phase properties to the choice of atomic polarizability parameters.

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Acknowledgments

The authors would like to thank the National Institutes of Health (NIH) for financial support (GM51501, GM07855) and Dr. Igor V. Vorobyov for helpful discussions and access to input scripts and results from previous simulations.

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Authors and Affiliations

  1. Department of Pharmaceutical Sciences, School of Pharmacy, University of Maryland Baltimore, Baltimore, MD, 21201, USA

    Christopher M. Baker & Alexander D. MacKerell Jr.

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  1. Christopher M. Baker
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  2. Alexander D. MacKerell Jr.
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Correspondence to Alexander D. MacKerell Jr..

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Baker, C.M., MacKerell, A.D. Polarizability rescaling and atom-based Thole scaling in the CHARMM Drude polarizable force field for ethers. J Mol Model 16, 567–576 (2010). https://doi.org/10.1007/s00894-009-0572-4

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  • DOI: https://doi.org/10.1007/s00894-009-0572-4

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