Yongjun Lü

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Name: Yongjun Lü
Organization: Tsinghua University
Department: School of Physics
Title:
Co-reporter:Yongjun Lü, Xiangxiong Zhang, and Min Chen
The Journal of Physical Chemistry B 2013 Volume 117(Issue 35) pp:10241-10249
Publication Date(Web):August 12, 2013
DOI:10.1021/jp404403k
The nucleation rate from classical nucleation theory is independent of sample size. In the past decades, several experimental and theoretical studies argued that the homogeneous nucleation rate of ice in supercooled droplets increases when the drop size is decreased. In this paper, we investigate the nucleation of ice in nanoscale water films using molecular dynamics simulations. We found that the nucleation rate of ice actually decreases when the film thickness decreases in the nanoscale regime. A theoretical model is presented to interpret the mechanism of nucleation rate decrease, which agrees well with the simulation results. The model divides films into the near-surface and the middle regions that are characterized by relatively low and high nucleation rates, respectively. The middle region dominates the nucleation process of films, whereas its effect is continuously weakened when increasing volume fraction of the near-surface region by decreasing the film size, leading to a decrease of the total nucleation rate. The structural and thermodynamic analyses indicate that the high stress induced by the surface layering slows down the diffusion and increases the nucleation barrier in the near-surface region, which is responsible for the low nucleation rate and eventually the decrease of the total nucleation rate.
Co-reporter:Yongjun Lü, Min Chen
Acta Materialia 2012 Volume 60(Issue 11) pp:4636-4645
Publication Date(Web):June 2012
DOI:10.1016/j.actamat.2012.03.038

Abstract

The crystallization of Ni90Si10 drops has been studied using molecular dynamics simulations. The atoms in the surface monolayer of the drop prematurely pack into a long-range ordered structure prior to volume crystallization, whereas diffusion dynamics maintains characteristic liquid-like features until the onset of volume crystallization. This surface crystallization process arises from strong density layering in the direction perpendicular to the drop surface. Due to density oscillations induced by the surface layering a high density state is produced in the drop surface, which is analogous to the effect of high pressure and locally increases the crystallization temperature of the surface layer, ultimately initiating crystallization from the surface. Such a layered structure causes pressure oscillation near the surface that produce a decrease in surface tension with decreasing temperature. The high density crystalline nature of the surface does not thermodynamically favor volume crystallization, which occurs separately via homogeneous nucleation in the interior with further decreasing temperature.