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Lewis-inspired representation of dissociable water in clusters and Grotthuss chains

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Abstract

Proton transfer to and from water is critical to the function of water in many settings. However, it has been challenging to model. Here, we present proof-of-principle for an efficient yet robust model based on Lewis-inspired submolecular particles with interactions that deviate from Coulombic at short distances to take quantum effects into account. This “LEWIS” model provides excellent correspondence with experimental structures for water molecules and water clusters in their neutral, protonated and deprotonated forms; reasonable values for the proton affinities of water and hydroxide; a good value for the strength of the hydrogen bond in the water dimer; the correct order of magnitude for the stretch and bend force constants of water; and the expected time course for Grotthuss transport in water chains.

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Acknowledgements

We thank Peter Jordan and Michael Francis Hagan for helpful discussions, Liliya Vugmeyster for guidance in Monte Carlo simulation, and Ercan Kamber for his advice regarding high performance computation. This work was supported by NIH grant R01EB001035.

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Author notes

  1. Stacy Dai

    Present address: Washington University School of Medicine, St. Louis, MO, 63110, USA

  2. Michael Blank

    Present address: Department of Chemistry, Stanford University, Palo Alto, CA, 94305, USA

Authors and Affiliations

  1. Graduate Program in Biophysics and Structural Biology, Brandeis University, Waltham, MA, 02454, USA

    Seyit Kale

  2. Department of Chemistry, Brandeis University, Waltham, MA, 02454, USA

    Judith Herzfeld, Stacy Dai & Michael Blank

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  1. Seyit Kale
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Correspondence to Judith Herzfeld.

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Kale, S., Herzfeld, J., Dai, S. et al. Lewis-inspired representation of dissociable water in clusters and Grotthuss chains. J Biol Phys 38, 49–59 (2012). https://doi.org/10.1007/s10867-011-9229-5

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