Investigating the mechanism of proton translocation in solution: from small chemical systems to biomolecules

在这项建议中概述的主要研究主题是质子转移反应在水溶液中使用计算方法的机制的调查。这些过程在许多化学和生物化学转化中起着重要作用，包括酸碱反应、酶催化、底物结合和能量传递。质子转移反应在散装水，在水和疏水介质之间的界面，以及在生物相关的系统的理论研究已经积极追求了至少二十年。然而，随着超快，时间分辨振动光谱技术的出现，上述质子转移过程可以第一次直接探测相关的空间和时间分辨率。这为计算化学提供了新的机会，有助于推进我们对质子转移反应的基本理解。

The major theme of research outlined in this proposal is the investigation of the mechanism of proton transfer reactions in aqueous solutions using computational approaches. These processes play a fundamental role in numerous chemical and biochemical transformations, including acid-base reactions, enzyme catalysis, substrate binding and energy transduction. Theoretical investigations of proton transfer reactions in bulk water, at the interface between aqueous and hydrophobic media, as well as in biologically-relevant systems have been actively pursued for at least two decades. However, with the recent advent of ultrafast, time-resolved vibration spectroscopy techniques, the aforementioned proton transfer processes can for the first time be directly probed with the relevant space and time resolution. This opens new opportunities for computational chemistry to contribute to the advancement of our fundamental understanding of proton transfer reactions.