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Revealing the role of liquid preordering in crystallisation of supercooled liquids

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  • Yuan-Chao Hu

    (University of Tokyo)

  • Hajime Tanaka

    (University of Tokyo
    University of Tokyo)

Abstract

The recent discovery of non-classical crystal nucleation pathways has revealed the role of fluctuations in the liquid structural order, not considered in classical nucleation theory. On the other hand, classical crystal growth theory states that crystal growth is independent of interfacial energy, but this is questionable. Here we elucidate the role of liquid structural ordering in crystal nucleation and growth using computer simulations of supercooled liquids. We find that suppressing the crystal-like structural order in the supercooled liquid through a new order-killing strategy can reduce the crystallisation rate by several orders of magnitude. This indicates that crystal-like liquid preordering and the associated interfacial energy reduction play an essential role in nucleation and growth processes, forcing critical modifications of the classical crystal growth theory. Furthermore, we evaluate the importance of this additional factor for different types of liquids. These findings shed new light on the fundamental understanding of crystal growth kinetics.

Suggested Citation

  • Yuan-Chao Hu & Hajime Tanaka, 2022. "Revealing the role of liquid preordering in crystallisation of supercooled liquids," Nature Communications, Nature, vol. 13(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-32241-z
    DOI: 10.1038/s41467-022-32241-z
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    References listed on IDEAS

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    1. Stefan Auer & Daan Frenkel, 2001. "Prediction of absolute crystal-nucleation rate in hard-sphere colloids," Nature, Nature, vol. 409(6823), pages 1020-1023, February.
    2. Mathieu Leocmach & Hajime Tanaka, 2012. "Roles of icosahedral and crystal-like order in the hard spheres glass transition," Nature Communications, Nature, vol. 3(1), pages 1-8, January.
    3. Li Zhong & Jiangwei Wang & Hongwei Sheng & Ze Zhang & Scott X. Mao, 2014. "Formation of monatomic metallic glasses through ultrafast liquid quenching," Nature, Nature, vol. 512(7513), pages 177-180, August.
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    Cited by:

    1. Zhao Fan & Hajime Tanaka, 2024. "Microscopic mechanisms of pressure-induced amorphous-amorphous transitions and crystallisation in silicon," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    2. Lu, Fenglian & Chen, Weiye & Hu, Shuzhi & Chen, Lei & Sharshir, Swellam W. & Dong, Chuanshuai & Zhang, Lizhi, 2024. "Achieving a smart thermal management for lithium-ion batteries by electrically-controlled crystallization of supercooled calcium chloride hexahydrate solution," Applied Energy, Elsevier, vol. 364(C).

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