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Published on: May 8, 2015
Ice Nucleation of Confined Monolayer Water Conforms to Classical Nucleation Theory
Zhuoran Qiao1, Yuheng Zhao1, Yi Qin Gao1
1Institute of Theoretical and Computational Chemistry, College of Chemistry and Molecular Engineering, Peking National Laboratory for Molecular Science , Peking University , Beijing 100871 , China.
Abstract:
We confirmed that monolayer water confined by parallel graphene sheets spontaneously crystallizes from a structurally and dynamically heterogeneous liquid phase under moderate supercooling via direct molecular dynamics simulation. Square-lattice-like geometric order is observed at the early stage of nucleation and is preserved during the entire nucleus growth process. The diffusion coefficient and free energy profile in the cluster space extracted from a Bayesian trajectory analysis agree well with the classical nucleation theory (CNT) prediction and yield thermodynamic quantities exhibiting linear temperature dependence. The effectiveness of maximum cluster size as the descriptor of ice nucleation dynamics in the CNT framework can be attributed to the dynamical time scale decoupling and strong structural pattern dependence of density fluctuation in the liquid phase.
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