文章基本信息

标题：Routes to cubic ice through heterogeneous nucleation
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作者：Michael Benedict Davies ; Martin Fitzner ; Angelos Michaelides 等
期刊名称：Proceedings of the National Academy of Sciences
印刷版ISSN：0027-8424
电子版ISSN：1091-6490
出版年度：2021
卷号：118
期号：13
页码：1
DOI：10.1073/pnas.2025245118
出版社：The National Academy of Sciences of the United States of America
摘要：The freezing of water into ice is one of the most important processes in the physical sciences. However, it is still not understood at the molecular level. In particular, the crystallization of cubic ice ( I c )—rather than the traditional hexagonal polytype ( I h )—has become an increasingly debated topic. Although evidence for I c is thought to date back almost 400 y, it is only in the last year that pure I c has been made in the laboratory, and these processes involved high-pressure ice phases. Since this demonstrates that pure I c can form, the question naturally arises if I c can be made from liquid water. With this in mind, we have performed a high-throughput computational screening study involving molecular dynamics simulations of nucleation on over 1,100 model substrates. From these simulations, we find that 1) many different substrates can promote the formation of pristine I c ; 2) I c can be selectively nucleated for even the mildest supercooling; 3) the water contact layer’s resemblance to a face of ice is the key factor determining the polytype selectivity and nucleation temperature, independent of which polytype is promoted; and 4) substrate lattice match to ice is not indicative of the polytype obtained. Through this study, we have deepened understanding of the interplay of heterogeneous nucleation and ice I polytypism and suggest routes to I c . More broadly, the substrate design methodology presented here combined with the insight gained can be used to understand and control polymorphism and stacking disorder in materials in general.
关键词：nucleation ; ice ; polymorphism ; molecular dynamics