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Critical-like behaviour of glass-forming liquids

Nature Materials volume 9, pages 324–331 (2010)Cite this article

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Abstract

Recently it has been revealed that when approaching the glass-transition temperature, Tg, the dynamics of a liquid not only drastically slows down, but also becomes progressively more heterogeneous. From our simulations and experiments of six different glass-forming liquids, we find that the heterogeneous dynamics is a result of critical-like fluctuations of static structural order, contrary to a common belief that it is purely of dynamic origin. The static correlation length and susceptibility of a structural order parameter show Ising-like power-law divergence towards the ideal glass-transition point. However, this structural ordering accompanies little density change, which explains why it has not been detected by the static structure factor so far. Our results suggest a far more direct link than thought before between glass transition and critical phenomena. Indeed, the glass transition may be a new type of critical phenomenon where a structural order parameter is directly linked to slowness.

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Figure 1: Structural order in glass-forming liquids.
Figure 2: Geometrical tiling patterns of 2DPC (Δ2DPC=9% and φ=0.73) and its φ dependence.
Figure 3: Spatial correlations of density and bond-orientational order.
Figure 4: The growth of medium-range crystalline order and its relation to the slow dynamics.
Figure 5: Finite-size scaling analysis of the criticality for 2DPC and 3DPC.
Figure 6: Critical-like behaviour of dynamics correlation in 2DPC (Δ2DPC=9%) and 3DPC (Δ3DPC=6%).

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Acknowledgements

The authors thank A. Furukawa for valuable discussion and C. Paddy Royall for a critical reading of the manuscript. This work was partially supported by a grant-in-aid from the Ministry of Education, Culture, Sports, Science and Technology, Japan.

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Authors and Affiliations

  1. Institute of Industrial Science, University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505, Japan

    Hajime Tanaka, Takeshi Kawasaki, Hiroshi Shintani & Keiji Watanabe

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  1. Hajime Tanaka
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  2. Takeshi Kawasaki
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Contributions

H.T. conceived and supervised the project, T.K. carried out simulations of 2DPC, 2DBL, 3DPC and 3DLJ, H.S. carried out simulations of 2DSL, K.W. carried out experiments of 2DGL, H.T. and T.K. analysed the data and H.T. wrote the manuscript.

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Correspondence to Hajime Tanaka.

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Tanaka, H., Kawasaki, T., Shintani, H. et al. Critical-like behaviour of glass-forming liquids. Nature Mater 9, 324–331 (2010). https://doi.org/10.1038/nmat2634

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