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Structural origin of enhanced slow dynamics near a wall in glass-forming systems

Nature Materials volume 10, pages 512–520 (2011)Cite this article

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Abstract

Spatial confinement is known to induce a drastic change in the viscosity, relaxation times, and flow profile of liquids near the glass (or jamming) transition point. The essential underlying question is how a wall affects the dynamics of densely packed systems. Here we study this fundamental problem, using experiments on a driven granular hard-sphere liquid and numerical simulations of polydisperse and bidisperse colloidal liquids. The nearly hard-core nature of the particle–wall interaction provides an ideal opportunity to study purely geometrical confinement effects. We reveal that the slower dynamics near a wall is induced by wall-induced enhancement of ‘glassy structural order’, which is a manifestation of strong interparticle correlations. By generalizing the structure-dynamics relation for bulk systems, we find a quantitative relation between the structural relaxation time at a certain distance from a wall and the correlation length of glassy structural order there. Our finding suggests that glassy structural ordering may be the origin of the slow glassy dynamics of a supercooled liquid.

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Figure 1: Effects of geometrical confinement on the structural relaxation time.
Figure 2: φ -dependence of the wall effects on the local structural relaxation time ταloc.
Figure 3: Structural and dynamic behaviour of 2DPL confined by rough walls and 2DBL confined by smooth walls.
Figure 4: 3DPL confined between two smooth flat walls.
Figure 5: Wall-induced structural ordering.
Figure 6: Layering near a wall and anisotropic particle motion.

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Acknowledgements

The authors are grateful to W. Kob for valuable discussions. This work was partly supported by a grant-in-aid from the Ministry of Education, Culture, Sports, Science and Technology, Japan and also by the Japan Society for the Promotion of Science (JSPS) through its FIRST Program.

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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

    Keiji Watanabe, Takeshi Kawasaki & Hajime Tanaka

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  1. Keiji Watanabe
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Contributions

H.T. conceived the project, K.W. performed granular experiments, T.K. performed numerical simulations, all authors analysed the data, and H.T. wrote the manuscript. K.W. and T.K. contributed equally to this work.

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Correspondence to Hajime Tanaka.

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Watanabe, K., Kawasaki, T. & Tanaka, H. Structural origin of enhanced slow dynamics near a wall in glass-forming systems. Nature Mater 10, 512–520 (2011). https://doi.org/10.1038/nmat3034

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