期刊
NATURE COMMUNICATIONS
卷 12, 期 1, 页码 -出版社
NATURE PORTFOLIO
DOI: 10.1038/s41467-021-25267-2
关键词
-
资金
- Hong Kong Research Grant Council [16302214, 16307718, 16303919, N_HKUST635/20, T13-605/18-W, AoE/M-09/12, AoE/P-705/16]
- Innovation and Technology Commission [ITCPD/17-9, ITC-CNERC14SC01]
- Hong Kong Research Grant Council Collaborative Research Fund [C6021-19EF]
The study uses Markov State Models and transition path theory to elucidate the ensemble pathways of heterogeneous ice nucleation. The results reveal that classical one-step and non-classical two-step nucleation pathways can co-exist at specific temperatures, with favorable conditions for the non-classical pathway. Insights into the mechanisms of heterogeneous ice nucleation are provided, shedding light on rational designs for controlling crystallization processes.
Ice nucleation on the surface plays a vital role in diverse areas, ranging from physics and cryobiology to atmospheric science. Compared to ice nucleation in the bulk, the water-surface interactions present in heterogeneous ice nucleation complicate the nucleation process, making heterogeneous ice nucleation less comprehended, especially the relationship between the kinetics and the structures of the critical ice nucleus. Here we combine Markov State Models and transition path theory to elucidate the ensemble pathways of heterogeneous ice nucleation. Our Markov State Models reveal that the classical one-step and non-classical two-step nucleation pathways can surprisingly co-exist with comparable fluxes at T = 230 K. Interestingly, we find that the disordered mixing of rhombic and hexagonal ice leads to a favorable configurational entropy that stabilizes the critical nucleus, facilitating the non-classical pathway. In contrast, the favorable energetics promotes the formation of hexagonal ice, resulting in the classical pathway. Furthermore, we discover that, at elevated temperatures, the nucleation process prefers to proceed via the classical pathway, as opposed to the non-classical pathway, since the potential energy contributions override the configurational entropy compensation. This study provides insights into the mechanisms of heterogeneous ice nucleation and sheds light on the rational designs to control crystallization processes. Classically, ice nucleation on foreign surfaces is considered a one-step process. Here, Li et al. uncover a two-barrier pathway which becomes competitive at lower temperatures, facilitated by synergistic, entropic effects of rhombic and hexagonal ice structures.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据