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Emergence of equilibrated liquid regions within the glass

Nature Physics volume 19, pages 114–119 (2023)Cite this article

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Abstract

The conventional understanding of the glass transition is that the transition from glass to liquid appears as a dynamic process in which atoms or molecules relax cooperatively into the equilibrium phase. Here we show that—in contrast to this picture—isolated regions of liquid form within the glassy matrix and the nature of the glass transition at a given temperature depends on the ratio between the relaxation time of the glass, τglass, and the alpha relaxation time of the equilibrated liquid, τα. At temperatures at which τglass/τα is large, we observe that high-mobility regions transit directly into the equilibrated liquid and subsequently grow by dynamic facilitation before—or while—cooperative glass relaxation sets into play. On the contrary, at temperatures associated with smaller τglass/τα, the glass transition proceeds by cooperative relaxation dynamics throughout the material. This behaviour is independent of the experimental procedure or protocol used to produce the glass.

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Fig. 1: Thermal protocol and samples under study.
Fig. 2: Glass transition in samples deposited at 0.99Tg.
Fig. 3: Glass transition in aged glasses.
Fig. 4: Glass transition in ultrastable glasses.

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Data that support the plots within this paper and other findings of this study are available from the corresponding authors upon reasonable request. Source data are provided with this paper.

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Acknowledgements

J.R.-V. and M.G.-S. acknowledge grant MAT2016-79759-R funded by MCIN/AEI/ 10.13039/501100011033 and ‘ERDF A way of making Europe’, and grant PID2020-117409RB-I00 funded by MCIN/AEI/10.13039/501100011033. C.R.-T. is a Serra Hunter Fellow. The ICN2 was funded by the CERCA programme/Generalitat de Catalunya. The ICN2 was supported by the Severo Ochoa Centres of Excellence Programme, funded by the Spanish Research Agency (AEI, grant no. SEV-2017-0706). All authors acknowledge Ll. Abad and IMB-CNM-CSIC for the fabrication of the nanocalorimeters.

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Authors and Affiliations

  1. Departament de Física, Facultat de Ciències, Universitat Autònoma de Barcelona, Bellaterra, Spain

    Ana Vila-Costa, Marta Gonzalez-Silveira, Cristian Rodríguez-Tinoco, Marta Rodríguez-López & Javier Rodriguez-Viejo

  2. Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and BIST, Bellaterra, Spain

    Ana Vila-Costa, Marta Gonzalez-Silveira, Cristian Rodríguez-Tinoco, Marta Rodríguez-López & Javier Rodriguez-Viejo

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Contributions

A.V.-C., M.G.-S. and J.R.-V. conceived and designed the experiments. A.V.-C. and M.R.-L. performed the experiments. All the authors contributed to the analysis of the data and discussed the results. M.G.-S., A.V.-C., C.R.-T. and J.R.-V. wrote the paper. M.G.-S. and J.R.-V. supervised the project.

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Correspondence to Marta Gonzalez-Silveira or Javier Rodriguez-Viejo.

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Supplementary Figs. 1 and 2 and Discussion.

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Source Data Fig. 2

Specific heat data and relaxation/transformation time.

Source Data Fig. 3

Specific heat data and relaxation/transformation time.

Source Data Fig. 4

Specific heat data and relaxation/transformation time.

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Vila-Costa, A., Gonzalez-Silveira, M., Rodríguez-Tinoco, C. et al. Emergence of equilibrated liquid regions within the glass. Nat. Phys. 19, 114–119 (2023). https://doi.org/10.1038/s41567-022-01791-w

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