Howard P. Isermann Department of Chemical & Biological Engineering, and Center for Biotechnology & Interdisciplinary Studies, Rensselaer Polytechnic Institute, Troy, New York 12180, USA.
J Phys Chem B. 2012 Mar 1;116(8):2498-503. doi: 10.1021/jp2107523. Epub 2012 Feb 16.
Water near extended hydrophobic surfaces is like that at a liquid-vapor interface, where fluctuations in water density are substantially enhanced compared to those in bulk water. Here we use molecular simulations with specialized sampling techniques to show that water density fluctuations are similarly enhanced, even near hydrophobic surfaces of complex biomolecules, situating them at the edge of a dewetting transition. Consequently, water near these surfaces is sensitive to subtle changes in surface conformation, topology, and chemistry, any of which can tip the balance toward or away from the wet state and thus significantly alter biomolecular interactions and function. Our work also resolves the long-standing puzzle of why some biological surfaces dewet and other seemingly similar surfaces do not.
靠近扩展的疏水表面的水类似于液体-蒸气界面处的水,在那里,与本体水中的密度涨落相比,水的密度涨落得到了极大的增强。在这里,我们使用具有特殊采样技术的分子模拟来表明,即使在复杂生物分子的疏水表面附近,水的密度涨落也同样得到了增强,这使它们处于去湿转变的边缘。因此,这些表面附近的水对表面构象、拓扑结构和化学性质的细微变化非常敏感,这些变化中的任何一种都可能使平衡向湿润状态或远离湿润状态倾斜,从而显著改变生物分子的相互作用和功能。我们的工作还解决了长期存在的难题,即为什么有些生物表面会去湿,而其他表面似乎相似却不会。