Kale Seyit, Herzfeld Judith, Dai Stacy, Blank Michael
Graduate Program in Biophysics and Structural Biology, Brandeis University, Waltham, MA 02454 USA.
J Biol Phys. 2012 Jan;38(1):49-59. doi: 10.1007/s10867-011-9229-5. Epub 2011 Jun 4.
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.
质子与水之间的相互转移在许多情况下对水的功能至关重要。然而，对其进行建模一直具有挑战性。在此，我们展示了一种基于受路易斯启发的亚分子粒子的高效且稳健模型的原理证明，该模型的相互作用在短距离内偏离库仑力，以考虑量子效应。这种“LEWIS”模型与中性、质子化和去质子化形式的水分子及水团簇的实验结构具有出色的一致性；给出了水和氢氧根质子亲和力的合理值；得出了水二聚体中氢键强度的良好值；给出了水的伸缩和弯曲力常数的正确量级；以及水链中质子迁移的预期时间进程。
