Zhang Weiwei, Chen Xing, van Duin Adri C T
Department of Mechanical and Nuclear Engineering , The Pennsylvania State University , University Park , Pennsylvania 16802 , United States.
Department of Chemistry , The Pennsylvania State University , University Park , Pennsylvania 16802 , United States.
J Phys Chem Lett. 2018 Sep 20;9(18):5445-5452. doi: 10.1021/acs.jpclett.8b02379. Epub 2018 Sep 10.
Investigating properties of both heavy and light water at the atomistic level is essential to understanding chemical and biological processes in aqueous solution. However, appropriately describing their difference on the nanoscale is still challenging. Employing ReaxFF reactive molecular dynamics simulations, we systematically study the structure, dynamics, and spectra of heavy and light water. With the water force field potential we developed, the different features between heavy and light water can be simulated appropriately by the classical treatment on large size and time scale. Here, we also report the structural difference between DO and HO in bulk heavy/light water. In addition, the diffusion constants of heavy and light water are successfully reproduced, and the Grotthuss hopping mechanism of proton transport in liquid water is properly described as well. It allows us to study a complex system in heavy/light aqueous environments, such as proton transport, chemical reaction, and tracing the reaction mechanism with an isotope substitute.
在原子水平上研究重水和轻水的性质对于理解水溶液中的化学和生物过程至关重要。然而，在纳米尺度上恰当地描述它们的差异仍然具有挑战性。利用ReaxFF反应分子动力学模拟，我们系统地研究了重水和轻水的结构、动力学和光谱。借助我们开发的水的力场势，重水和轻水之间的不同特征可以通过在大尺寸和时间尺度上的经典处理得到适当模拟。在此，我们还报告了重水/轻水主体中DO和HO之间的结构差异。此外，成功再现了重水和轻水的扩散常数，并且正确描述了液态水中质子传输的Grotthuss跳跃机制。这使我们能够研究重水/轻水体系中的复杂系统，如质子传输、化学反应以及用同位素替代物追踪反应机理。
