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Asymmetric caging in soft colloidal mixtures

Nature Materials volume 7, pages 780–784 (2008)Cite this article

Abstract

The long-standing observations that different amorphous materials exhibit a pronounced enhancement of viscosity and eventually vitrify on compression or cooling continue to fascinate and challenge scientists1, on the ground of their physical origin and practical implications. Glass formation is a generic phenomenon, observed in physically quite distinct systems that encompass hard and soft particles. It is believed that a common underlying scenario2,3, namely cage formation, drives dynamical arrest, especially at high concentrations. Here, we identify a novel, asymmetric glassy state in soft colloidal mixtures, which is characterized by strongly anisotropically distorted cages, bearing similarities to those of hard-sphere glasses under shear. The anisotropy is induced by the presence of soft additives. This phenomenon seems to be generic to soft colloids and its origins lie in the penetrability of the constituent particles. The resulting phase diagram for mixtures of soft particles is clearly distinct from that of hard-sphere mixtures and brings forward a rich variety of vitrified states that delineate an ergodic lake in the parameter space spanned by the size ratio between the two components and by the concentration of the additives. Thus, a new route opens for the rational design of soft particles with desired tunable rheological properties.

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Figure 1: Experimental and MCT arrested state diagrams for star–star mixtures.
Figure 2: Rheological properties for star–star mixtures from experiments and MCT calculations.
Figure 3: Dynamical properties of star–star mixtures based on numerical simulations.
Figure 4: Structural properties of star–star mixtures and visualization of the asymmetric cages, based on numerical simulations.

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Acknowledgements

Helpful discussions with J. Roovers are gratefully acknowledged. This work has been supported by the Marie Curie Network on Dynamical Arrest of Soft Matter and Colloids MRTNCT-2003-504712, the NoE SoftComp NMP3-CT-2004-502235 and the DFG through the SFB TR6. C.M. acknowledges financial support by the Alexander von Humboldt Foundation.

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Author notes

  1. E. Stiakakis

    Present address: Present address: Forschungszentrum Jülich, Weiche Materie, D-52425 Jülich, Germany,

Authors and Affiliations

  1. Dipartimento di Fisica and CNR-INFM-SOFT, Università di Roma La Sapienza, I-00185 Rome, Italy

    C. Mayer, E. Zaccarelli & F. Sciortino

  2. Institut für Theoretische Physik II: Weiche Materie, Heinrich-Heine-Universität, D-40225 Düsseldorf, Germany

    C. Mayer, C. N. Likos & H. Löwen

  3. FO.R.T.H., Institute of Electronic Structure and Laser, GR-71110 Heraklion, Crete, Greece

    E. Stiakakis & D. Vlassopoulos

  4. The Erwin Schrödinger International Institute for Mathematical Physics (ESI), Boltzmanngasse 9, A-1040 Vienna, Austria

    C. N. Likos

  5. Department of Chemistry, Institute for Polymer Research, University of Waterloo, ON, N2L 3G1, Canada

    A. Munam & M. Gauthier

  6. Department of Chemistry, University of Athens, GR-15771 Athens, Greece

    N. Hadjichristidis & H. Iatrou

  7. Dipartimento di Fisica and CNR-INFM-SMC, Università di Roma La Sapienza, I-00185 Rome, Italy

    P. Tartaglia

  8. Department of Materials Science and Technology, University of Crete, GR-71003 Heraklion, Crete, Greece

    D. Vlassopoulos

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  1. C. Mayer
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Correspondence to C. Mayer or E. Zaccarelli.

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Mayer, C., Zaccarelli, E., Stiakakis, E. et al. Asymmetric caging in soft colloidal mixtures. Nature Mater 7, 780–784 (2008). https://doi.org/10.1038/nmat2286

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