Using Activation Energies to Elucidate Mechanisms of Water Dynamics
Using Activation Energies to Elucidate Mechanisms of Water Dynamics
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DOI：
10.1021/acs.jpca.1c08020
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发表时间：
2021-11-25
影响因子：
2.9
通讯作者：
Thompson, Ward H.
中科院分区：
文献类型：
--
作者：
Piskulich, Zeke A.;Laage, Damien;Thompson, Ward H.
在计算活化能方面的最新进展为液态水的动态时间尺度提供了新的线索。在这个角度下，我们研究了激活能如何解释氢键(H键)伙伴的交换在重排水的H键网络中的中心作用，但不是单一的作用。讨论了其他运动对动力学时间尺度的贡献及其相关的活化能，同时讨论了振动光谱扩散的一种情况，其中氢键交换不具有机械意义。对悬而未决的挑战的新进展，包括对非阿累尼乌斯效应和激活量的描述，以及未来调查的一些方向，都有详细的说明。
Recent advances in the calculation of activation energies are shedding new light on the dynamical time scales of liquid water. In this Perspective, we examine how activation energies elucidate the central, but not singular, role of the exchange of hydrogen-bond (H-bond) partners that rearrange the H-bond network of water. The contributions of other motions to dynamical time scales and their associated activation energies are discussed along with one case, vibrational spectral diffusion, where H-bond exchanges are not mechanistically significant. Nascent progress on outstanding challenges, including descriptions of non-Arrhenius effects and activation volumes, are detailed along with some directions for future investigations.