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Elastic ripening and inhibition of liquid–liquid phase separation

Nature Physics volume 16, pages 422–425 (2020)Cite this article

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Abstract

Phase separation is a central concept of materials physics1,2,3 and has recently emerged as an important route to compartmentalization within living cells4,5,6. Biological phase separation features activity7, complex compositions8 and elasticity9, which reveal important gaps in our understanding of this universal physical phenomenon. Here, we explore the impact of elasticity on phase separation in synthetic polymer networks. We show that compressive stresses in a polymer network can suppress phase separation of the solvent that swells it, stabilizing mixtures well beyond the liquid–liquid phase-separation boundary. Network stresses also drive a new form of ripening, driven by transport of solute down stiffness gradients. This elastic ripening can be much faster than conventional Ostwald ripening driven by surface tension.

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Fig. 1: Network stiffness controls droplet nucleation.
Fig. 2: Stiffness gradients drive solute transport and ripening.
Fig. 3: Rate of ripening increases with stiffness difference.

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Data availability

The data represented in Figs. 1b and 3 are available as Source Data. All other data that support the findings of this study are available from the corresponding author on reasonable request.

Code availability

The code that supports the findings of this study is available from the corresponding author on reasonable request.

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Acknowledgements

We acknowledge the Swiss National Science Foundation, National Centre of Competence in Research ‘Bio-Inspired Materials’ for funding, as well as L. Wilen, S. Kumar and T. Cohen for helpful discussions.

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Author notes

  1. These authors contributed equally: Kathryn A. Rosowski, Tianqi Sai.

Authors and Affiliations

  1. Department of Materials, ETH Zürich, Zürich, Switzerland

    Kathryn A. Rosowski, Tianqi Sai, Robert W. Style & Eric R. Dufresne

  2. Max Planck Institute for Dynamics and Self-Organization, Göttingen, Germany

    Estefania Vidal-Henriquez & David Zwicker

Authors
  1. Kathryn A. Rosowski
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  2. Tianqi Sai
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  3. Estefania Vidal-Henriquez
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  4. David Zwicker
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  5. Robert W. Style
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  6. Eric R. Dufresne
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Contributions

T.S. and K.A.R., under the supervision of R.W.S. and E.R.D., designed, performed, analysed and interpreted the experiments. E.V.-H., under the supervision of D.Z., performed the numerical simulations. E.R.D., K.A.R. and R.W.S. wrote the paper with contributions from E.V.-H. and D.Z.

Corresponding authors

Correspondence to Robert W. Style or Eric R. Dufresne.

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The authors declare no competing interests.

Additional information

Peer review information Nature Physics thanks Christoph Weber and the other, anonymous, reviewer(s) for their contribution to the peer review of this work.

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Extended Data Fig. 1 Saturation concentration is independent of Young’s modulus.

The saturation volume fraction of fluorinated oil in silicone gels of four different stiffnesses, at \(4{0}^{\circ }\)C.

Extended Data Fig. 2 Quench rate dependence of nucleation temperature.

The nucleation temperature of samples with the same stiffness (680 kPa) and different quench rates.

Supplementary information

Supplementary Information

Supplementary Figs. 1–13, methods, legends for videos, and references.

Supplementary Video 1

Time evolution of droplets on the soft side (10 kPa) of the gradient, far from the interface.

Supplementary Video 2

Time evolution of droplets on the stiff side (700 kPa) of the gradient, far from the interface.

Supplementary Video 3

Time evolution of droplets at the interface of the gradient.

Supplementary Video 4

Time evolution of two droplets of different sizes in a homogeneous gel.

Supplementary Video 5

Average droplet radius profile over time for experiment and simulation, with E = 750 kPa and using simulation parameters γ = 4.4 nN m−1 and δ = 40 μm.

Source data

Source Data Fig. 1b

Source data for figure 1, panel b

Source Data Fig. 3

Source data for figure 3, panels a–c, d

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Rosowski, K.A., Sai, T., Vidal-Henriquez, E. et al. Elastic ripening and inhibition of liquid–liquid phase separation. Nat. Phys. 16, 422–425 (2020). https://doi.org/10.1038/s41567-019-0767-2

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