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Bibliographic Details
Main Authors: Guo, Jianqing, Zhou, Liying, Zen, Andrea, Michaelides, Angelos, Wu, Xifan, Wang, Enge, Xu, Limei, Chen, Ji
Format: Preprint
Published: 2020
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Online Access:https://arxiv.org/abs/2009.04727
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Table of Contents:
  • Understanding the hydration and diffusion of ions in water at the molecular level is a topic of widespread importance. The ammonium ion (NH$_4^+$) is an exemplar system that has received attention for decades because of its complex hydration structure and relevance in industry. Here we report a study of the hydration and the rotational diffusion of NH$_4^+$ in water using ab initio molecular dynamics simulations and quantum Monte Carlo calculations. We find that the hydration structure of NH$_4^+$ features bifurcated hydrogen bonds, which leads to a rotational mechanism involving the simultaneous switching of a pair of bifurcated hydrogen bonds. The proposed hydration structure and rotational mechanism are supported by existing experimental measurements, and they also help to rationalize the measured fast rotation of NH$_4^+$ in water. This study highlights how subtle changes in the electronic structure of hydrogen bonds impacts the hydration structure, which consequently affects the dynamics of ions and molecules in hydrogen bonded systems.