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Sussman DM, Schoenholz SS, Cubuk ED, et al. Disconnecting structure and dynamics in glassy thin films. Proc Natl Acad Sci U S A. 2017;114(40):10601-10605doi: 10.1073/pnas.1703927114.
Sussman, D. M., Schoenholz, S. S., Cubuk, E. D., & Liu, A. J. (2017). Disconnecting structure and dynamics in glassy thin films. Proceedings of the National Academy of Sciences of the United States of America, 114(40), 10601-10605. https://doi.org/10.1073/pnas.1703927114
Sussman, Daniel M, et al. "Disconnecting structure and dynamics in glassy thin films." Proceedings of the National Academy of Sciences of the United States of America vol. 114,40 (2017): 10601-10605. doi: https://doi.org/10.1073/pnas.1703927114
Sussman DM, Schoenholz SS, Cubuk ED, Liu AJ. Disconnecting structure and dynamics in glassy thin films. Proc Natl Acad Sci U S A. 2017 Oct 03;114(40):10601-10605. doi: 10.1073/pnas.1703927114. Epub 2017 Sep 19. PMID: 28928147; PMCID: PMC5635874.
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Proc Natl Acad Sci U S A. 2017 Oct 03;114(40):10601-10605. doi: 10.1073/pnas.1703927114. Epub 2017 Sep 19.

Disconnecting structure and dynamics in glassy thin films.

Proceedings of the National Academy of Sciences of the United States of America

Daniel M Sussman, Samuel S Schoenholz, Ekin D Cubuk, Andrea J Liu

Affiliations

  1. Department of Physics, Syracuse University, Syracuse, NY 13244; [email protected].
  2. Google Brain, Google, Mountain View, CA 94043.
  3. Department of Materials Science and Engineering, Stanford University, Stanford, CA 94304.
  4. Department of Physics and Astronomy, University of Pennsylvania, Philadelphia, PA 19104.

PMID: 28928147 PMCID: PMC5635874 DOI: 10.1073/pnas.1703927114

Abstract

Nanometrically thin glassy films depart strikingly from the behavior of their bulk counterparts. We investigate whether the dynamical differences between a bulk and thin film polymeric glass former can be understood by differences in local microscopic structure. Machine learning methods have shown that local structure can serve as the foundation for successful, predictive models of particle rearrangement dynamics in bulk systems. By contrast, in thin glassy films, we find that particles at the center of the film and those near the surface are structurally indistinguishable despite exhibiting very different dynamics. Next, we show that structure-independent processes, already present in bulk systems and demonstrably different from simple facilitated dynamics, are crucial for understanding glassy dynamics in thin films. Our analysis suggests a picture of glassy dynamics in which two dynamical processes coexist, with relative strengths that depend on the distance from an interface. One of these processes depends on local structure and is unchanged throughout most of the film, while the other is purely Arrhenius, does not depend on local structure, and is strongly enhanced near the free surface of a film.

Keywords: glass; machine learning; thin film

Conflict of interest statement

The authors declare no conflict of interest.

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