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Ultrastable monodisperse polymer glass formed by physical vapour deposition

Nature Materials volume 19, pages 1110–1113 (2020)Cite this article

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Abstract

Stable glasses prepared by vapour deposition are an analogue of glassy materials aged for geological timescales. The ability to prepare such materials allows the study of near-ideal glassy systems. We report the preparation and characterization of stable glasses of polymers prepared by physical vapour deposition. By controlling the substrate temperature, deposition rate and polydispersity, we prepared and characterized a variety of stable polymer glasses. These materials display the kinetic stability, low fictive temperatures and high-density characteristic of stable glasses. Extrapolation of the measured transformation times between the stable and normal glass provides estimates of the relaxation times of the equilibrium supercooled liquid at temperatures as much as 30 K below the glass transition temperature. These results demonstrate that polymer stable glasses are an exciting and powerful tool in the study of ultrastable glass and disordered materials in general.

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Fig. 1: Thickness change versus temperature for the initial and subsequent heating and cooling cycles of various kinetically stable glasses.
Fig. 2: MALDI-TOF data for polymers in different phases of stable glass production.
Fig. 3
Fig. 4: Estimating relaxation times for stable glass films of PS.

Data availability

The datasets generated during and/or analysed during the current study are available in the UW Dataverse repository at https://doi.org/10.5683/SP2/YBVEMX. Source data are provided with this paper.

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Acknowledgements

The authors acknowledge discussions with M. Ediger and Z. Fakhraai. Financial support from Natural Sciences and Research Council of Canada is gratefully acknowledged. Research at Perimeter Institute is supported by the Government of Canada through Industry Canada and by the Province of Ontario through the Ministry of Economic Development and Innovation. J.A.F. thanks the ESPCI for funding through the Paris Sciences Chair program.

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Authors and Affiliations

  1. Department of Physics & Astronomy, University of Waterloo, Waterloo, Ontario, Canada

    Adam N. Raegen, Junjie Yin & James A. Forrest

  2. Perimeter Institute for Theoretical Physics, Waterloo, Ontario, Canada

    Junjie Yin & James A. Forrest

  3. Department of Physics & Astronomy and Department of Chemistry, University of Waterloo, Waterloo, Ontario, Canada

    Qi Zhou

  4. School of Science, Beijing Jiaotong University, Beijing, China

    Qi Zhou

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  1. Adam N. Raegen
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  2. Junjie Yin
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  4. James A. Forrest
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Contributions

A.N.R. performed experiments, data analysis and contributed to the writing and editing of the manuscript. J.Y. and Q.Z. performed experiments, data analysis and contributed to the editing of the manuscript. J.A.F. conceived the experiments, contributed to data analysis, wrote the draft manuscript and contributed to the editing of the manuscript.

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Correspondence to James A. Forrest.

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Supplementary information

Supplementary Information

Supplementary Figs. 1–7, methods and discussion.

Source data

Source Data Fig. 1

Thickness versus temperature data used in Fig. 1.

Source Data Fig. 2

Histogram data from MALDI

Source Data Fig. 3

Density data for Tg–Tf.

Source Data Fig. 4

Transformation kinetics data.

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Raegen, A.N., Yin, J., Zhou, Q. et al. Ultrastable monodisperse polymer glass formed by physical vapour deposition. Nat. Mater. 19, 1110–1113 (2020). https://doi.org/10.1038/s41563-020-0723-7

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