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Time reversibility during the ageing of materials

Nature Physics volume 20, pages 637–645 (2024)Cite this article

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Abstract

Physical ageing is the generic term for irreversible processes in glassy materials resulting from molecular rearrangements. One formalism for describing such ageing processes involves the concept of material time, which may be thought of as time measured on a clock whose rate changes as the glass ages. Experimental determination of material time has so far not been realized, however. Here we show how dynamic light-scattering measurements provide a way forward. We determined the material time for an ageing sample of the glass-former 1-phenyl-1-propanol after temperature jumps close to the glass transition from the time-autocorrelation function of the intensity fluctuations probed by multispeckle dynamic light scattering. These fluctuations are shown to be stationary and reversible when regarded as a function of the material time. The glass-forming colloidal synthetic clay Laponite and a chemically ageing curing epoxy are also shown to display material-time-reversible scattered-light intensity fluctuations, and simulations of an ageing binary system monitoring the potential energy confirm material-time reversibility. In addition to demonstrating direct measurements of the material time, our findings identify a fundamental property of ageing in quite different contexts that presents a challenge to the current theories of ageing.

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Fig. 1: Multispeckle DLS.
Fig. 2: Verifying the triangular relation.
Fig. 3: Determining and validating the material time for down jumps to 193 K.
Fig. 4: Stationarity and reversibility of the intensity fluctuations regarded as functions of the material time.
Fig. 5: Physical ageing data for the colloidal glass-former Laponite, chemical ageing data for a linear polymerizing epoxy and computer simulation data for a binary LJ system.

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Data availability

The study generated ∼10 TB of data, which are available from the corresponding authors upon request.

Code availability

The code for the analysis of all data sets is available from the corresponding authors upon request.

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Acknowledgements

We thank M. Zanin and S. Ditlevsen for advice regarding the data analysis. This work was supported by the VILLUM Foundation’s Matter grant (VIL16515) and by the Deutsche Forschungsgemeinschaft (grants BL 923/1 and BL 1192/3).

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Authors and Affiliations

  1. Institute for Condensed Matter Physics, Technical University of Darmstadt, Darmstadt, Germany

    Till Böhmer, Jan-Niklas Kociok & Thomas Blochowicz

  2. Glass and Time, IMFUFA, Department of Science and Environment, Roskilde University, Roskilde, Denmark

    Jan P. Gabriel, Lorenzo Costigliola, Tina Hecksher & Jeppe C. Dyre

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  1. Till Böhmer
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Contributions

J.C.D. and T. Blochowicz devised the project; T. Böhmer and J.P.G. planned the experiments; T. Böhmer, J.P.G. and J.-N.K. performed the experiments; T. Böhmer and J.P.G. analysed the experimental data; L.C. and T. Böhmer performed and analysed the computer simulations; T.H., J.C.D. and T. Blochowicz supervised the experiments and data analysis, T. Böhmer and J.C.D. wrote the paper with input from all authors; J.C.D. and T. Blochowicz provided resources and acquired funding.

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Correspondence to Till Böhmer, Jeppe C. Dyre or Thomas Blochowicz.

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Böhmer, T., Gabriel, J.P., Costigliola, L. et al. Time reversibility during the ageing of materials. Nat. Phys. 20, 637–645 (2024). https://doi.org/10.1038/s41567-023-02366-z

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