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Visualizing kinetic pathways of homogeneous nucleation in colloidal crystallization

Nature Physics volume 10, pages 73–79 (2014)Cite this article

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Abstract

When a system undergoes a transition from a liquid to a solid phase, it passes through multiple intermediate structures before reaching the final state. However, our knowledge on the exact pathways of this process is limited, mainly owing to the difficulty of realizing direct observations. Here, we experimentally study the evolution of symmetry and density for various colloidal systems during liquid-to-solid phase transitions, and visualize kinetic pathways with single-particle resolution. We observe the formation of relatively ordered precursor structures with different symmetries, which then convert into metastable solids. During this conversion, two major cross-symmetry pathways always occur, regardless of the final state and the interaction potential. In addition, we find a broad decoupling of density variation and symmetry development, and discover that nucleation rarely starts from the densest regions. These findings hold for all of our samples, suggesting the possibility of finding a unified picture for the complex crystallization kinetics in colloidal systems.

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Figure 1: Structures of nuclei and precursors in early crystallization.
Figure 2: Kinetic pathways during crystallization.
Figure 3: Local density evolution throughout crystallization.

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Acknowledgements

P.T. and L.X. are supported by the Research Grants Council of Hong Kong (GRF grant CUHK404211, ECS grant CUHK404912, CUHK Direct Grant 4053021), and N.X. is supported by the National Natural Science Foundation of China (No. 91027001 and 11074228), the National Basic Research Program of China (973 Program No. 2012CB821500), the CAS 100-Talent Program (No. 2030020004), and Fundamental Research Funds for the Central Universities (No. 2340000034). We thank H. Tanaka and E. Sloutskin for helpful discussions, and A. Schofield for providing the particles.

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Authors and Affiliations

  1. Department of Physics, The Chinese University of Hong Kong, Hong Kong, China

    Peng Tan & Lei Xu

  2. Hefei National Laboratory for Physical Sciences at Microscale and Department of Physics, CAS Laboratory of Soft Matter Chemistry, University of Science and Technology of China, Hefei 230026, China

    Ning Xu

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  1. Peng Tan
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Contributions

P.T. and L.X. conceived and designed the experiments, P.T. performed the experiments, P.T., N.X. and L.X. analysed the data, P.T. developed the new approach of local bond order analysis, and P.T. and L.X. wrote the paper.

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Correspondence to Lei Xu.

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Tan, P., Xu, N. & Xu, L. Visualizing kinetic pathways of homogeneous nucleation in colloidal crystallization. Nature Phys 10, 73–79 (2014). https://doi.org/10.1038/nphys2817

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