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Dynamical Heterogeneity in a Vapor-Deposited Polymer Glass



Jack F. Douglas, Wengang Zhang, Francis W. Starr


Recently, there has been great interest in 'ultrastable' glasses formed via vapor deposition, both because of emerging applications of these materials (e.g., active layers in light-emitting diodes and photovoltaics) and, theoretically, as materials for probing equilibrium properties of glassy mate-rials below their glass transition, based on the assumption that these materials are “equivalent” to glassy materials aged over astronomical timescales. We use molecular simulations to contrast thermodynamic, structural, and dynamic properties of vapor-deposited and ordinary quenched glasses. While our simulated ultrastable glasses reproduce the expected trends in the thermodynamic properties of these films, such as a higher density and lower potential energy than ordinary glasses, the relaxation times of the ultrastable and ordinary glasses are nearly the same when com-pared at the same temperature. This observation is clearly inconsistent with the proposition that the ultrastable glasses are equivalent to highly-aged glasses. The stability of vapor-deposited films results from the polymers being trapped in a highly non-equilibrium state, as in isolated strongly adsorbed polymers on substrates and solution-deposited multi-layer polyelectrolyte films.
Journal of Chemical Physics


ultrastable glass, vapor deposition, glass formation, enthalpy, density, relaxation time, non-equilibrium state


Douglas, J. , Zhang, W. and Starr, F. (2017), Dynamical Heterogeneity in a Vapor-Deposited Polymer Glass, Journal of Chemical Physics (Accessed May 21, 2024)


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Created February 23, 2017, Updated April 23, 2020