Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 112, Issue 27, Pages 8227-8231Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1503133112
Keywords
glass transition; cooperative rearrangement; thin films
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Funding
- Natural Sciences and Engineering Research Council of Canada
- Perimeter Institute for Theoretical Physics
- Government of Canada through Industry Canada
- Province of Ontario through the Ministry of Economic Development Innovation
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We introduce a minimal theory of glass formation based on the ideas of molecular crowding and resultant string-like cooperative rearrangement, and address the effects of free interfaces. In the bulk case, we obtain a scaling expression for the number of particles taking part in cooperative strings, and we recover the Adam-Gibbs description of glassy dynamics. Then, by including thermal dilatation, the Vogel-Fulcher-Tammann relation is derived. Moreover, the random and string-like characters of the cooperative rearrangement allow us to predict a temperature-dependent expression for the cooperative length. of bulk relaxation. Finally, we explore the influence of sample boundaries when the system size becomes comparable to.. The theory is in agreement with measurements of the glass-transition temperature of thin polymer films, and allows quantification of the temperature-dependent thickness h(m) of the interfacial mobile layer.
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