文献类型：期刊文献

英文题名：Time-dependent density functional theory for the freezing/melting transition in interfacial systems

作者：Liu, Yu[1,2];Guo, Fangyuan[1,3];Hu, Jun[1,3];Liu, Honglai[1,3];Hu, Ying[1,3]

机构：[1]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Sch Chem Engn, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China

年份：2019

卷号：207

起止页码：327

外文期刊名：CHEMICAL ENGINEERING SCIENCE

收录：;EI(收录号：20192607113008);WOS:【SCI-EXPANDED(收录号:WOS:000481644300025)】；

基金：Yu Liu and Fangyuan Guo contributed equally to this work. This work is sponsored by the National Natural Science Foundation of China (No. 21776070, 91534202, 91834301), and the Shanghai Rising Star Program (19QA1402400).

语种：英文

外文关键词：Freezing; Time-dependent density functional theory; Interface; Nano-droplet; Crystal

摘要：We propose a three-dimensional time-dependent density functional theory (TDDFT) to investigate the freezing/melting of Lennard-Jones fluids in interfacial systems including flat interfaces and nano-droplets. The theory is based on a modified fundamental measure theory (MFMT) for the hard-sphere reference system plus mean field theory (MFT) for the attractive contributions plus an additional weighted density approximation (WDA) contribution to enforce that bulk liquid equation of state is that of modified Benedict, Webb and Rubin (MBWR). By using different initial states, our theory generated a series of equilibrium structures including crystals and polyhedral particles. The non-linear effect and the irreversibility of the freezing/melting process were captured. The profiles for free energy and the order parameter indicate that the free energy barrier existing in the freezing/melting process is caused by the break in symmetry. Additionally, the time-dependent properties were also examined, and provided insight into the mechanism of the freezing process. (C) 2019 Published by Elsevier Ltd.