New Insights into the Role of Water in Biological Function: Studying Solvated Biomolecules Using Terahertz Absorption Spectroscopy in Conjunction with Molecular Dynamics Simulations

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• 作者：Valeria Conti Nibali ; Martina Havenith
• 刊名：Journal of the American Chemical Society
• 出版年：2014
• 出版时间：September 17, 2014
• 年：2014
• 卷：136
• 期：37
• 页码：12800-12807
• 全文大小：554K
• ISSN：1520-5126

文摘

In life science, water is the ubiquitous solvent, sometimes even called the 鈥渕atrix of life鈥? There is increasing experimental and theoretical evidence that solvation water is not a passive spectator in biomolecular processes. New experimental techniques can quantify how water interacts with biomolecules and, in doing so, differs from 鈥渂ulk鈥?water. Terahertz (THz) absorption spectroscopy has turned out to be a powerful tool to study (bio)molecular hydration. The main concepts that have been developed in the recent years to describe the underlying solute-induced sub-picosecond dynamics of the hydration shell are discussed herein. Moreover, we highlight recent findings that show the significance of hydrogen bond dynamics for the function of antifreeze proteins and for molecular recognition. In all of these examples, a gradient of water motion toward functional sites of proteins is observed, the so-called 鈥渉ydration funnel鈥? By means of molecular dynamics simulations, we provide new evidence for a specific water鈥損rotein coupling as the cause of the observed dynamical heterogeneity. The efficiency of the coupling at THz frequencies is explained in terms of a two-tier (short- and long-range) solute鈥搒olvent interaction.